Citation
Excitation and ionization of gases by fission fragments.

Material Information

Title:
Excitation and ionization of gases by fission fragments.
Creator:
Walters, Roy Alan, 1941-
Publication Date:
Language:
English
Physical Description:
xv, 308 leaves. : ill. ; 28 cm.

Subjects

Subjects / Keywords:
Argon ( jstor )
Cathodes ( jstor )
Electrons ( jstor )
Energy ( jstor )
Gases ( jstor )
Glow discharges ( jstor )
Helium ( jstor )
Ions ( jstor )
Lasers ( jstor )
Plasmas ( jstor )
Ionization of gases ( lcsh )
Nuclear excitation ( lcsh )
Genre:
bibliography ( marcgt )
theses ( marcgt )
non-fiction ( marcgt )

Notes

Thesis:
Thesis--University of Florida.
Bibliography:
Bibliography: leaves 302-307.
General Note:
Typescript.
General Note:
Vita.
Statement of Responsibility:
By Roy Alan Walters.

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Source Institution:
University of Florida
Holding Location:
University of Florida
Rights Management:
Copyright [name of dissertation author]. Permission granted to the University of Florida to digitize, archive and distribute this item for non-profit research and educational purposes. Any reuse of this item in excess of fair use or other copyright exemptions requires permission of the copyright holder.
Resource Identifier:
022768312 ( ALEPH )
ADA8623 ( NOTIS )
14039068 ( OCLC )
AA00004931_00001 ( sobekcm )

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Full Text















EXCITATION AND IONIZATION OF GASES

BY FISSION FRAGMENTS














By

ROY ALAN WALTERS


A DI-:.ERi'AT:ON PRESENTED TO THP GRADUATE COUNCIL OF
THE 'UN-VERSI't'l OF FIORIDA IN PARTIAL
FULPILM[INT 01 TIhL : ;Cr- 1 F'.-L NTS FOR THE DEGREE OF
DOCTOR OF PHBLOSOP, I




INI'VL'PSITY OF FLORIDA
197 9




EXCITATION AND IONIZATION OF GASES
BY FISSION FRAGMENTS
By
ROY ALAN WALTERS
4 DISSERTATION PRESENTED TO THE GRADUATE COUNCIL OF
THE UNIVERSITY OF FLORIDA IN PARTIAL
FULFILLMENT 01 THE REQUIREMENTS FOR THE DEGREE OF
DOCTOR OF PHILOSOPHY
UNIVERSITY OF FLORIDA
1973


bL-IZ-Z
To my father,
Harry Walters,
who was, in my eyes, the greatest of
engineers and the greatest of men.


ACKNOWLEDGMENTS
The author would like to express his deepest appreciation and
gratitude to Dr. Richard T. Schneider, the chairman of his supervisory
committee, for his guidance and support in this research, and for the
faith and friendship he showed toward the author throughout this
academic endeavor. Sincere thanks are extended to the other members
of the supervisory committee, Drs. Hugh D. Campbell, Kwan Chen, George
R. Dalton, and William H. Ellis.
The author also wishes to thank Dr. Edward Carroll for his
ideas and encouragement on the LMFBR detector studies.
Special note should be made of the valuable contributions of
Mr. Ernest Whitman, who aided the author with the design and construc
tion of the vacuum chamber, and of Mr. Richard Paternoster, who
developed the computer analysis and plotting programs. Thanks are
also extended to Mr. George Wheeler for his valuable assistance in the
construction of equipment and its operation.
The author acknowledges the technical assistance provided by
Mr. Henry Gogun and the other members of the UFTR crew.
Special thanks are extended to the author's wife and son for
their help in the production of this paper and for their patience and
support through the years this endeavor has taken to complete.
The author will be forever indebted to his father, the late
Harry Walters, for his unfailing faith and encouragement, and most
iii


especially, for his aid in the actual production of this manuscript.
Many of the diagrams that are a part of this dissertation are products
of his highly skilled hands.
Appreciation is expressed to Mrs. Edna Larrick for typing the
final draft of this manuscript.
This research was supported by NSA Grant NGL-10-005-089.
IV


TABLE OF CONTENTS
Page
ACKNOWLEDGMENTS iii
LIST OF TABLES viii
LIST OF FIGURES ix
ABSTRACT xiii
CHAPTER
1 INTRODUCTION 1
1.1 The Nuclear-Pumped Laser 1
1.2 Previous Studies of Fission
Fragment-Produced Plasmas . 9
1.3 Glow Discharge Irradiation and Fission Fragment
Interaction Experiments 11
2 THEORETICAL CONSIDERATIONS 14
2.1 Energy Deposition by Fission Fragments
and Other Particles 14
2.2 Energy Deposition by the Reaction He^(n,p)T
in a Glow Discharge 37
2.3 Description of a Fission Fragment-Produced Plasma 40
3 PLASMA RESEARCH APPARATUS 49
3.1 Introduction 49
3.2 Primary System 50
3.2.1 Plasma Region 51
3.2.2 Vacuum Chamber; Optical, Gas
and Electrical Feeds 55
3.3 Uranium Coatings 57
3.3.1 Coating Requirements 57
3.3.2 Coating Thickness 57
3.3.3 Review of Methods and Chemistry 60
3.3.4 Chemical Procedures 61
3.3.5 Mechanical Coating Procedure 63
v


TABLE OF CONTENTS (Continued)
CHAPTER Page
3 (Continued)
3.4 Support Systems 65
3.4.1 Reactor: Neutron Flux and Gamma Dose 65
3.4.2 Electrical Systems 67
3.4.3 Gas Filling Systems 68
3.4.4 Shielding 70
3.4.5 Safety 71
3.5 Data Acquisition Systems 75
4 ANALYSIS OF "iN-REACTOR" PLASMAS: FISSION FRAGMENT
GENERATED AND GLOW DISCHARGE 77
4.1 Experimental Procedure and Data Analysis:
Fission Fragment Interactions 78
4.2 Helium 86
4.2.1 Helium Kinetics and Spectral Analysis 88
4.2.2 Line Intensity and Excited State Density ... 92
4.2.3 Boltzmann Plot Analysis 102
4.2.4 Field Amplification of Line Intensities .... 110
4.3 £rgon Excitation by Fission Fragments 121
4.3.1 Argon Kinetics and Spectral Analysis 122
4.3.2 Line Intensity and Excited State Density . 131
4.3.3 Boltzmann Plot Analysis 135
4.3.4 Field Amplification 140
4.4 CF^ Fission Fragment Interactions 153
4.5 Glow Discharge Irradiations 160
4.5.1 Experimental Procedures 161
4.5.2 The Glow Discharge 161
4.5.3 General Reactor Mixed Radiation Effects
on the Glow Discharge 164
4.5.4 Volume Deposition 171
4.5.5 Cathode Deposition 174
5 APPLICATIONS OF FISSION FRAGMENT-PRODUCED PLASMAS .... 178
5.1 The Nuclear-Pumped Laser 179
5.2 A Neutron Detector for the Liquid Metal
Fast Breeder Reactor 187
5.2.1 Diagnostic and Power Supply Systems 190
5.2.2 Neutron Detector Experimental Results 192
5.2.3 Data Projections and Realistic Chamber Design 198
vi


TABLE OF CONTENTS (Continued)
CHAPTER Page
6 CONCLUSIONS 201
APPENDIX
I PRESSURE DEPENDENCE OF RELATIVE LINE INTENSITIES
AND EXCITED STATE DENSITIES HELIUM 205
II BOLTZMANN TEMPERATURE PLOTS HELIUM 223
III PRESSURE DEPENDENCE OF RELATIVE LINE INTENSITIES
AND EXCITED STATE DENSITIES ARGON 231
IV BOLTZMANN TEMPERATURE PLOTS ARGON 277
V FIELD AMPLIFICATION OF ARGON SPECTRAL EMISSION 295
BIBLIOGRAPHY 302
BIOGRAPHICAL SKETCH 308
vii


LIST OF TABLES
Table Page
4-1 HELIUM DATA 116
4-2 IDENTIFIED CASCADES OF ARGON II 134
4-3 ARGON DATA 145
4-4 CF FISSION FRAGMENT IRRADIATIONS:
BAND PEAKS OBSERVED AT 760 TORR 160
viii


LIST OF FIGURES
Figure Page
2-1 Geometry 21
2-2 Range of Fission Fragments in Helium and Argon 29
2-3 Deposition of Energy into Helium by Fission Fragments,
§ = 3.8 x 1011 ^ 33
cm -sec
2-4 Deposition of Energy into Argon by Fission Fragments,
$ = 3.8 x 1011 ~ 34
cm -sec
2-5 Energy Deposition by Fission Fragments in Argon
and Helium A Fixed Cavity 36
3-1 Reactor Mounting 52
3-2 Chamber Experimental Sections 53
3-3 Chamber Detail Reactor Region 54
3-4 University of Florida Training Reactor 56
3-5 K as a Function of Density 58
3-6 The Kinetic Energy of Fission Fragments as
a Function of Mass Number [38] 59
3-7 Chemical Procedures Coating Solution 62
3-8 Mechanical Procedures for Coating 64
3-9 Distribution of Thermal Neutron Flux
along Experimental Chamber 66
3-10 General Gas Discharge I-V Characteristic 69
3-11 Chamber Mounting and Shielding Cave 72
4-1 Helium Spectrum 79
'4-2 Helium Spectrum 80
xx


LIST OF FIGURES (Continued)
Figure Page
4-3 Helium Spectrum 81
4-4 Helium Spectrum 82
4-5 Helium Spectrum 83
4-6 Helium Excited States and Transitions 87
4-7 Optically Viewed Energy Deposition in Helium
and Argon as a Function of Pressure 95
4-8 Helium Intensity and Energy Deposition as
a Function of Pressure 97
4-9 Relative Excited State Population Density as
a Function of Pressure 98
4-10 Line Intensity versus Pressure Helium 99
4-11 Boltzmann Plot Helium Glow Discharge 104
4-12 Boltzmann Plot Fission Fragment Excited Helium .... 105
4-13 Pressure Dependence of the Boltzmann Plot
Correlation Coefficients Helium 107
4-14 Boltzmann Temperature as a Function of Pressure 108
4-15 Current-Voltage Characteristics of
Fission Fragment Excited Helium 112
4-16 Line Amplification and Current as a Function of
Applied Voltage 30.5 cm Long Helium Cavity 114
4-17 Electron Energy Distribution Fission Fragment
Excited Helium 120
4-18 Argon Spectrum 124
4-19 Argon Spectrum 125
4-20 Argon Spectrum 126
4-21 Argon Spectrum 127
4-22 Argon Spectrum 128
4-23 Argon Spectrum 129
x


LIST OF FIGURES (Continued)
Figure Page
4-24 Intensity and Calculated Deposition (Viewed)
as a Function of Pressure 133
4-25 Boltzmann Temperature Plot 600 torr Argon I 137
4-26 Boltzmann Plot Argon II, 600 torr 138
4-27 Argon Temperature and Correlation Coefficient
versus Pressure 139
4-28 Amplification and Current versus Applied Voltage -
150 torr Argon 141
E
4-29 Amplification Coefficient versus , Argon 143
4-30 Electron Density and Temperature versus Pressure Argon 148
4-31 Ion Pair Generation Rate as a Function
of Pressure Argon 149
4-32 Electron Energy Distribution Argon 151
4-33 Electron Energy Distribution Argon 152
4-34 Glow Discharge through 5.5 torr CF^ 2000 A - 5087 A . 155
4-35 Band Peak Intensity of 100 torr CF4 as a Function of Time 156
4-36 Spectrum of Fission Fragment Excited CF^,
760 torr 2000 A 5087 A 158
4-37 Spectrum of Fission Fragment Excited CF^,
760 torr 2646 A 3280 A 159
3
4-38 Glow Discharge I-V Characteristics for He -CO -N ,
8:1:1, 10 torr 165
4-39 I-V Characteristics for Hollow Cathode Glow Discharges . 167
4-40 I-V Characteristics, 3.3 torr Glow Discharge,
Flat Cathode 168
4-41 Voltage Decay, Glow Discharge, for Reactor Shutdown -
Constant 1, 20 ma 169
4-42 Voltage Decay, Glow Discharge, for Reactor Shutdown -
Hollow Cathode 170
xi


LIST OF FIGURES (Continued)
Figure
5-1 Nuclear Pumped Laser
5-2 Nuclear-Pumped Laser Output
5-3 Cavity Design
5-4 LMFBR Neutron Detector Signal Flow
5-5 Amplification of Argon Line Intensity versus
Reactor Power
O
5-6 Ar I 6965 A Filtered Output Neutron Detector
5-7 Total Spectrum Signal Neutron Detector .
Page
181
184
186
191
194
195
196
5-8
P-P Voltage versus Reactor Power Neutron Detector
197


Abstract of Dissertation Presented to the
Graduate Council of the University of Florida in Partial
Fulfillment of the Requirements for the Degree of Doctor of Philosophy
EXCITATION AND IONIZATION OF GASES
BY FISSION FRAGMENTS
By
Roy Alan Walters
June, 1973
Chairman: Dr. Richard T. Schneider
Major Department: Nuclear Engineering Sciences
The excitation and ionization produced by fission fragments was
investigated to identify basic mechanisms that could be applied to
direct nuclear pumping or enhancement of gas lasers.
A cylindrical U foil and its axial electrodes were placed
00
in a vacuum chamber which was capable of transmission of fluorescence to
o o
its exterior from 2000 A to 8000 A. The chamber was filled with argon,
helium or carbon tetrafluoride at various pressures and emersed in
11 2
a thermal neutron flux of 3.8 y 10 n/cm -sec.
The spectrum obtained from this excitation was qualitatively
similar to a glow discharge for argon and helium except for the pres
ence of excited ion species of He II and Ar III. The spectral output
from irradiation of 760 torr carbon tetra fluoride provided a band
system that is presently unidentified. Pressure dependent relative
intensity and excited state density data provide information on state
and species kinetics such as formation of molecular ions and their loss
Four possible population inversions were identified in
xi ii
mechanisms.


Ar II. Boltzmann analysis of the excited states supplied a temperature
for each species where the correlation coefficients of the fit lines
indicate that the plasmas are typical nonequilibrium cascade systems.
10-3
Electron densities around 10 e /cm and Maxwellian temperature
values for the collected electrons have been obtained from the recombina
tion region I-V characteristics. Electron energy distributions formu
lated from the data compare favorably with referenced calculations.
Ion pair generation rates were well within expected deviation compared
to calculations using a two-region energy deposition model.
In the ion chamber region of the I-V characteristics, line
emission increased as an exponential function of field strength.
A model for this amplification was developed for argon, utilizing an
amplification coefficient applicable to all pressures.
A neutron detector was developed for the liquid metal fast
breeder reactor by using optical transmission from the reactor core of
electric field modulated emission from fission fragment excitation.
Measurement of the modulated field effect eliminates the majority of
noise sources and gamma degradation signal loss associated with other
detectors.
Because of the excellent spectral output from Ar II, a nuclear
pumped argon ion optical cavity was constructed. Data from reactor
irradiation of the cavity indicate that it was lasing.
The effect of mixed radiation from the reactor on a glow dis-
11
charge was studied. For thermal neutron fluxes less than 3.8 X 10
2 7 3
n/cm -sec and gamma dose rates of 1.1 x 10 R/hr, irradiations of He ,
4
He N and mixtures thereof show that there is no volume deposition
xiv


effect on the glow discharge. A cathode photoemission effect was found
that altered the balance of the discharge. Positive ion bombardment
3
from the He (n,p)T reaction products produced a considerable electron
source that perturbed the cathode fall region. Enhancement of CC>2 lasers
was shouai to be a mechanism of preionization for low voltage glow dis
charge initiation and subsequent maintenance with lower power input.
This lowers the temperature of the discharge and improves laser pumping
efficiency.
xv


CHAPTER 1
INTRODUCTION
During the last decade, fission fragments and other energetic
heavy ions that are produced by neutron reactions have been examined
as possible sources of energy for generation of high temperature plas
mas. These high energy particles can be produced in great numbers in
a nuclear reactor where the reaction source (neutron flux) can range
17 2
up to 10 n/cm -sec in short pulses. The main thrust of research in
this area has been toward the demonstration of a nuclear-pumped laser.
1.1 The Nuclear-Pumped Laser
The term "Nuclear-Pumped Laser" refers to a laser that is
excited by products of nuclear reactions only and not by any electri
cal or optical source.
The link between the reactor and laser is natural when one
considers that communications could be greatly aided with transmission
of data to earth by laser beam in advanced extraterrestial equipment
which will have to include a nuclear reactor for power generation.
Direct coupling of a laser to a nuclear reactor is necessary
in order to produce desired high input powers. One might envision
a reactor-laser system where an optical cavity and the reactor fuel
235
are combined. A set of U internally coated tubes could be grouped
together in a cylindrical shape where the optical cavity would be
1


2
formed by mirrors reflecting through the tubes. A neutron moderator
would surround the tubes and cooling could be accomplished by passing
the laser gas through the tubes and then through a heat exchanger.
235
The fissioning of the U would supply both neutrons for sustaining
the nuclear reaction and fission fragments for excitation of the gas.
Each fission event supplies two fission fragments, a heavy fragment
with an average energy of 67.5 MeV and a light fragment with an aver
age energy of 98.7 MeV. These light and heavy fragments vary in weight
according to the familiar fission product distribution, but both frag
ments have the very important characteristic of being emitted with
a charge of about 20 e. This results in a very large coulombic inter
action rate and, thus, a very large deposition of energy in a small
path length, producing the excited states utilized in the laser.
Operating this reactor in a pulse mode will maximize the peak laser
power output.
Another nuclear-pumped laser scheme involves a gas core reactor
using UF as a fuel and some fluoride molecular species derived from
6
UF dissociation reactions as the lasing species. A similar homogen-
6
235
eous concept involves insertion of U compounds into a liquid dye
laser in order to produce a critical mass and thus a reactor. This
system would derive its excitation from fission fragments rather than
from chemical or optical sources. One disadvantage of the liquid dye
laser concept is the apparent breakdown of long chain dye molecules by
radiation interaction. R. Schneider [ 1 ] has inserted Rotemin b dis
solved in ethyl alcohol into a reactor and observed fluorescence.


3
When the dye was removed from the reactor, it was evident that it had
been completely destroyed, since there was no color, or fluorescence,
left in the liquid. Much experimental work has been done trying to
show the feasibility of a nuclear-pumped laser. To date, no proof has
been presented that confirms the operation of such a laser.
There are several alternatives when considering an energy
source for direct excitation of a laser. The most widely available
source is gamma radiation, but in order to effect efficient energy
transfer, high density solids must be used. A desire to optimize the
absorption led early workers [2,3] to concentrate on direct excitation
of solid state lasers. However, gamma radiation was found to suppress,
rather than aid, lasing action in all solids studied to date. This
"cutoff" phenomenon is generally attributed to radiation damage in the
solid.
An obvious solution to the problem of radiation damage is to
use a gas or liquid lasing medium. For gases, this implies the use of
a high energy heavy particle that has a large dE/'dx. Such a particle
is exemplified by the fission fragment. Liquid lasers are still in
their infancy and only one published report is available on an attempt
at nuclear pumping [4]. Nuclear pumping of gas lasers has been studied
extensively starting with a comprehensive study by L. Herwig [5] xn
1964. He recognized the radiation damage problem associated with
solids and decided to concentrate on gas laser nuclear pumping.
His calculations showed that He-Ne laser threshold requirements were
theoretically within the reach of some reactor and accelerator radiation


4
sources. Herwig also noted that a large diameter laser may be possible
due to the inherently low electron temperature expected in the radia
tion produced plasma.
J. DeShong [6] carried out more detailed calculations and
showed that a high pressure, large diameter nuclear-pumped laser has
theoretical efficiency two orders of magnitude greater than small diam
eter devices. In 1967 he undertook a series of experiments to verify
the feasibility of direct pumping. None of his devices showed proof of
lasing. Eerkins [7,8] decided to study noble gases as a possible lasing
medium because their high density allows a large dE/dx by the fission
fragment and because their ionization energy is low (E^ = 15.68 eV for
argon). Because recombination and dissociative recombination is ex
tremely efficient in a cold plasma, it was felt that the argon ion tran
sitions would exhibit a population inversion greater than that seen in
conventional electrically pumped lasers. Eerkins's source of energy
17 2
was a TRIGA pulsed reactor with fluxes up to 10 n/cm -sec. The
235
reactor neutrons interacted with a U coating on the laser tube wall
and produced a fission fragment-generated plasma. Boron-coated walls
10 7
were also tried, using the reaction B (n.oOLi producing a plasma
utilizing the reaction product energy of 2.3 MeV. Although Eerkins
did not find any proof of lasing, he did generate a light output that
was quite intense. Guyot [9], concentrating on Ar and C02 lasers, also
did not find lasing in his experiments.
Nuclear-pumped laser experiments previously mentioned concen
trated on pumping with a highly energetic particle that was a result


5
of a neutron reaction with B or a fission event. These experiments
also concentrated the reacting material on tube walls while inserting
gas as a target for the particles. V. Andriakhin [10] attempted lasing
in an entirely different manner. He utilized the large neutron cross
3 3
section (5000b) of the He reaction [He (n,p)T + 760 keV] to provide
3
a source for excitation in a cavity filled with a gas mixture of He
and mercury vapor. His device generated light output of 10 mW, but no
proof of lasing was seen.
Several researchers (T. Ganley [11], F. Allario [121, H. Rhoads
[13]) noted the inability of others to generate a nuclear-pumped laser
and decided to look at the effects of several nuclear sources on an
3
operating laser. All of these studies involved the use of He as a
4
replacement for He in a He-C02~N2 laser gas mixture while operating
the laser in a nuclear reactor. It was felt that the high efficiency
3
of the C02 laser would allow maximum conversion of the He (n,p)T reac
tion energy, 760 keV, into laser output.
All three authors noted an increase in the efficiency of the
laser being irradiated in the reactor and, therefore, an increase in
laser output. Rhoads recognized this increased laser efficiency as an
increase of the glow discharge efficiency. He described this effect
as primarily due to the bombardment of the cathode surface by gammas
and He (n,p)T reaction products and thus an alteration in the cathode
O
fall equilibrium. The output of a C02 laser depends, among other
things, on the electron temperature, Te, of the plasma. Bullis [14]
has shown that the electron temperature for optimum pumping of a C02


6
laser is far below that resulting from normal glow discharge pumping.
The addition of the radiation source term to the cathode fall equilib
rium allows the operation of a glow discharge at much lower currents
and field strengths, allowing lower Te and much more efficient pumping.
This irradiation effect also allows operation of glow discharges at
much higher pressures than previously attainable.
It would also be possible to increase the power output of
present operating laser systems by the addition of a radiation source
at the cathode.
The glow discharge irradiation work described in this disserta
tion was done simultaneously with the nuclear-enhanced laser work de
scribed above; the results shown in this paper basically agree with
those described above.
Upon termination of the nuclear-pumped laser experiments, it
became evident that the theoretical considerations used to calculate
the neutron flux needed for lasing action may be inaccurate. The
thermal flux level available in many reactors is well above the calcu
lated lasing thresholds; therefore, some of the experimental devices
should have lased. Most of the theoretical work has been based on the
premise that one excited state is available for each 100 eV deposited
in the gas [5,6], This relation results from the assumption that once
the energy is deposited in a gas by nuclear interactions, subsequent
distribution of excited states, ionization, etc., is identical to that
of electrically pumped lasers.


7
G. R. Russell [15,16] has noted at least for the case of
atomic argon direct nuclear excitation of gases is an entirely dif
ferent kinetic process than that found in most CW electrically excited
lasers. Generally, in electrically pumped gas lasers population inver
sions are formed by metastable state collisions with ground state atoms
(He-Ne) or other energy transfer systems initiated by the electron
swarm.
The kinetics of the argon ion laser, where the population
inversion is produced by electron collisional excitation of the upper
state and electron recombination in the lower state, served as Russell's
example. On the average, it takes two collisions with electrons to
elevate the argon ground state to the ionized excited level required
for population inversion. Such a ladder-climbing system is not evident
in the low temperature plasma generated by nuclear sources. This low
temperature system is more analogous to a recombining plasma at low
thermal electron temperatures, where there is additional preferential
excitation due to high energy particles superimposed on the thermal
excitation. Therefore, it would not be expected that inversions formed
in electrically excited CW lasers would necessarily be found in nuclear-
excited lasers. It is also very probable that the additional excita
tion due to high energy heavy particles will create new inversions not
previously observed in electrically excited lasers.
Russell supports this last premise by calculating population
inversions produced in argon by fission fragment interactions and not
available in conventionally pumped lasers. His calculations included


8
formation of excited states due to recombination of thermal electrons
and the associated radiative and collisional decay of these states.
To complicate matters further, Miley [17] and others have indicated
that there is a difference between how fission fragments and alpha
particles lose their energy in a gas medium. This is because alpha
particles remain essentially charge invariant over their path length,
while fission fragments starting with an average charge of 20e lose
their charge by recombination while losing energy by coulombic, rather
than nuclear, elastic collisions. Recently several of the authors [ 1]
mentioned above have revealed that they now feel that once the fission
fragment deposits its energy into a gas, this excited gas may be
regarded as identical to the electrically excited gas.
From the above discussion it can be concluded that the exact
nature of a gas excited by fission fragments is not known. Also, there
is a distinct possibility of producing a nuclear-pumped laser using
some unusual (not normally available) population inversion; some gas
now known to exhibit population inversions may become the standard for
this type of laser. A less optimistic conclusion is that nuclear
pumping is not presently feasible.
No one has previously studied experimentally the excited
states of a plasma produced by an extremely large source of heavy,
highly charged particles such as fission fragments. Until detailed
analysis of heavy particle-produced plasmas is complete, the nuclear-
pumped laser experiments are without foundation.


9
1.2 Previous Studies of Fission
Fragment-Produced Plasmas
To study excited states of atomic and ionized species exper
imentally, spectrographic analysis of the spontaneous photon emission
from these states is necessary.
Several researchers have studied experimentally alpha particle-
induced luminescence of gases with great success. S. Dondes et al. [18]
have been able to supply very good spectrographic plates (long time
210
exposures) of many gases exposed to a Po ,5 MeV, alpha source.
Amplification of the gross light output was indicated upon placing a
350 V/'cm field across the luminescing area. P. Thiess [19] using
a similar but more powerful source and photon counting techniques,
was able to obtain similar data. Other allied work has come from the
French gas counter research program [2o,21,22,2 3] and two very early
studies [24,2 5], These latter experimental works used sources of very
low intensity and the data were decidedly biased toward use in the
design of counting equipment. The source strengths used in all of
the alpha particle interaction work are weak enough, and the electron
density therefore small enough, that the gas should probably be described
as a scintillating light source rather than a plasma. As mentioned
previously, it is hard to draw comparisons between such low level
a source luminescence and a plasma generated by a large fission frag
ment source, but these studies do give basic knowledge of the kinetics
of heavy particle interactions.
In contrast to excited state measurements, fairly extensive
measurements of electron densities in radiation-produced plasmas have


10
been reported. Jamerson et al. [26,27] worked with "in-reactor" fission
fragment-produced plasmas where, utilizing the I-V curves produced by
a field across the plasma, they were able to calculate values for
12 2
electron temperature and density. For a flux of 10 n/cm -sec a 600K
electron temperature was found which compares favorably with the micro-
wave cavity measurements of Bhattacharya [28]. Ellis et al. [29,30,31],
3
have studied recombination coefficients in plasmas produced by He reac
tion products, alpha particles, and fission fragments, and have added
immensely to the knowledge of the kinetics of these plasmas.
The above works indicate that the general kinetics studies of
alpha and fission fragment-produced plasmas are no longer in their
infancy; therefore, one can draw' on these data in explaining the source
terms for generating atomic excited states.
A very large library of cross sections for collision-produced
excited states is available in a book by E. W. Thomas [32]. These
cross sections have been generated by bombarding various gases by heavy
ions produced in accelerators. Unfortunately, none of the ions had
energies above 1.5 MeV and few had energies above 0.5 MeV. The appli
cability of these cross section data to fission fragment interactions is
questionable, but certain techniques used to generate these data are
of great interest in this study.
Several researchers have attempted to study spectral emissions
from fission fragment plasmas. F. Morse et al. [33] studied the
luminescence of several gases under bombardment by fission fragments
in a nuclear reactor. They did see some line structure, but concluded


11
that it was too weak to study (96-hour exposures!). They then returned
to the use of alpha sources [18] where reactor associated problems were
not present. R. Axtmann [34] studied the luminescent intensity of
252
nitrogen bombarded by fission fragments from Cf but he just assumed
that the light was from the second positive system of molecular nitro
gen emission and tried no spectroscopic analysis. The above studies
led Pagano [35] to attempt spectroscopic analysis of various gases
252
bombarded by Cf fission fragments, but his source was not strong
enough to allow recording of spectra.
During the nuclear-pumped laser studies of Eerkins [7,8],
several spectroscopic plates of their pulsed plasma were taken, but
at that time they were more interested in producing a laser than study
ing the plasma that they assumed contained population inversions.
Thus, the spectroscopic work was limited to a few plates in which the
photon output was filtered by the mirrors of the laser system.
The above spectroscopic studies gave great encouragement to
this author in his studies of "in-core" fission fragment-produced
plasmas. After careful analysis of the techniques used by these
researchers, a set of experimental guidelines (see Chapter 3) were
generated in order to avoid the known problems associated with such
research.
1.3 Glow Discharge Irradiation and
Fission Fragment Interaction Experiments
The need for experimental data on fission fragment-produced
plasmas and on the radiation-produced changes in an already existing
plasma has been established. The dual purpose of this dissertation


12
is to fill some of this unknown area and to generate sound techniques
for the study of "in-reactor" particle produced plasmas. Fortunately,
as will be shown in the following chapters, one basic experimental
apparatus can be used for this dual purpose.
The first probe into this area involves the study of a known
plasma, the glow discharge, and what happens to its operation under
3
bombardment by gamma and reaction products of the He (n,p)T reaction.
Several cathode configurations and several gases are studied for their
response to the reactor sources. Conclusions are drawn as to the extent
of changes and how they occur.
The most difficult area, the investigation of fission fragment-
produced excitation, is presented utilizing the assumption that the
plasma is an interacting Maxwellian system. The analysis of the data
emphasizes the deviations from equilibrium of this system. This approach
was taken due to the availability of large numbers (45 Ar II spectral
lines) of easily measurable spectral lines emitted by atomic as well as
4
ion species of several gases. He Ar, and CF^ were studied for pos
sible population inversions by using Boltzmann plot techniques and
analysis of deviations of excited state populations as a function of
pressure. Data are supplied on the effect of pressure and a DC field
on the intensity of line emission.
A unique neutron detector for the liquid metal fast breeder
reactor was suggested by Dr. Edward E. Carroll [36]. Drawing from the
above data, a detection system was developed and tested using electric
field amplified light variations as a basis for its operation. Also,
an argon ion laser was tested utilizing pumping by fission fragment


13
interactions only. Results from this device, although not proof of las
ing, show promise for future investigators.
In summary, this chapter has outlined the great need for
experimental data on the nature of effects of mixed radiation sources
on a glow discharge and has shown why the study of fission fragment-
produced plasmas is necessary.


CHAPTER 2
THEORETICAL CONSIDERATIONS
To assess adequately the effects observed in the experimental
procedure, certain theoretical considerations must be made. The two
basic considerations that will be reviewed in this chapter are, first,
the way a particle deposits its energy, and, second, how this energy
might be distributed in a plasma. Basic calculational techniques will
also be reviewed for use in analysis of the data described later in
this study.
2.1 Energy Deposition by Fission Fragments
and Other Particles
The passage of charged particles through matter has been
studied for at least half a century. It is not surprising that the
theoretical and experimental description of alpha-particle and proton
penetration phenomena is well advanced as these are the charged particles
with which most experiments were performed before the discovery of nu
clear fission. Presently there is emphasis on the study of the inter
action of ions with larger mass and charge than these elemental par
ticles. It is common practice to label ions such as fission fragments
as "heavy ions in order to distinguish them from light ions such as
protons and alpha particles. This distinction is strictly arbitrary
since most of the phenomena involved in energy deposition by these
14


15
particles are identical. Fission fragments distinguish themselves as
heavy ions because they are very massive and have, immediately after
formation, about twenty electrons stripped from their atoms. Thus, the
effective charge of these fragments is considerably higher than those
of the light ion group. This is an important distinction, since heavy
ions suffer coulombic interactions, as well as the nuclear elastic
scattering found in light ion interactions. A light ion is essentially
charge invariant over its path length, while the fission fragment is
charge variable over part of its path.
The life of a fission fragment or other heavy particle is
summarized by Northcliffe [37]. If an atom is given a velocity greatly
in excess of the orbital velocities of its electrons and allowed to
enter a material medium, these electrons will be stripped from the atom
and the bare nucleus will proceed through the medium, gradually losing
energy because of coulornbic interactions with the electrons of the
medium. At this point, where the heavy particle velocity is high,
elastic or inelastic collisions with the nuclei of the medium will be
relatively rare and will add little to the energy loss process. At
first there is a small, but finite, probability that the ion will cap
ture an electron in one of these collisions and a large probability
that the electron will be lost in the next collision; but as the ion
slows down and approaches velocities comparable with the orbital veloc
ity of a captured electron, the capture probability increases and the
loss probability decreases. As the ion slows to velocities smaller
than the orbital velocity of the first captured electron, the capture
probability becomes very large and the loss probability approaches zero.


16
Meanwhile the probability of capturing a second electron grows and the
corresponding loss probability decreases, so that with increasing prob
ability the second electron is retained. As the velocity decrease con
tinues, a third electron is captured in the same gradual way, and then
a fourth, and so on. The major difference in the description of the
capture process for successive electrons is the change in velocity
scale necessary to match the progressive decrease of orbital velocity
of these electrons within the ion.
Eventually the ion reaches velocities smaller than the orbital
velocity of the least tightly bound electron and spends most of its
time as a neutral atom. By this time its kinetic energy is being
dissipated predominately by the energy transfer arising from elastic
collisions between the screened nuclear fields of the ion and atom,
and a diminishing amount of energy is being transferred to the atomic
electrons. The neutralized ion is said to be stopped when it either
reaches thermal velocities or combines chemically with the atoms of the
stopping material.
With respect to the medium into which the heavy particle or
fission fragment is penetrating, most of the ionization and excita
tion is caused by secondary electrons (delta rays) produced during the
initial coulombic stripping and recombination interactions. This does
not hold true, though, for a fission fragment near the end of its track,
where it is essentially neutral.
To calculate the space dependent deposition of energy in a
medium, it is usual to start with a stopping power relation. Using
appropriate geometry, one first calculates the available energy per


17
unit volume, and then using ion or excited state generating terms, the
kinetics of the system. The Bohr stopping equation for fission frag
ments is [3 8]
" S = 2TTNZeff ~^~2 Le + 2ttNZiZ2 ~2 Lv
mv
m2v
(1)
where
_ rot {3 -1/3 1 -1
L = L ( x + x
e e \4 4
- (hhvr (Â¥ J2
N = atom density of the density stopping material
M^,Z = mass and nuclear charge of the moving fragment
M ,Z = mass and nuclear charge of the stopping material
Cj Z
e,m = electronic charge and mass
v = velocity of the moving fragment
effective charge of the fission fragment example:
Z
eff
l/3 .
. .. = Z v/v
eff o
.8
v =
x =
L =
L =
velocity of a Bohr-orbit electron (2.2 x 10 cm/sec)
v
2Z
eff v
term for electronic stopping power
term for nuclear stopping power
L = the electronic stopping power for a particles of comparable
e
-8
velocities (about 6.33 x 10 v).


18
The first term in the right-hand side of equation (1) describes
the electronic stopping power derived from coulombic interactions.
The second term describes energy transfer by nuclear elastic inter
actions. It is standard practice to ignore the second term since the
amount of energy deposited by nuclear interactions is small compared
to the total energy deposited. Thus, using the first term only of
equation (1), the range of a fission fragment can be determined.
1 2
Assuming for the particle that E = M v and that the Thomas-Fermi
& X
1/3
effective charge, Z ^ = Z v/vq, is va]-icl> the fragment velocity
follows from equation (1) as
dv
dx
K(N,Z1,M1) ,
where
K(N,Z1,M1)
= 2rrN
4 -8
e 6.33 x 10
,1/3
mv
8M-
6Z
.2/9
.1/3
+ 1
(2)
(3)
K is therefore a function of the mass and charge of the moving
fragment and the density of the medium, but is velocity and space inde
pendent. Solving this equation shows that
v(x) = v. Kx .
(4)
Solving this velocity-distance relationship for x when
v(x) = 0 or v(x)i = 0, where R equals the range of a particle
I x=R
with initial velocity v the result is
R(v. )
i
v.
i
IT
(5)


19
Assuming the initial energy = M^v^ and substituting into
equation (4) produces the well-known square law energy deposition rela
tionship of a fission fragment,
E(x) = E.(1 £)2 (6)
1 I
This relationship is therefore equivalent to the Bohr stopping
power equation using the Thomas-Fermi approximation for Z __ with the
efx
nuclear stopping term neglected.
Several authors' using the general equation,
E = E.(1 £) (7)
1 K
have disagreed with the n=2 value derived above. Axtmann [34], using
the luminescence of nitrogen under fission fragment bombardment, found
n equal to 1.7. Long [39] used n= 1 for his calculations where the
n value was obtained from collated range-energy data for a variety of
stopping materials. Steele [40] used n=1.5 to compute energy deposi
tion by fission fragments in water.
To generalize the square law equation (6) for a point source
in an infinite homogeneous medium, an energy transfer function can be
stated as
G(x, p) = E. (1 )
l pR
(8)
where cos p is the angle between the x-axis and the direction of
particle movement.
To calculate the deposition in a gas by a fission fragment,
one must remember that a fission fragment source such as a coating of


20
U0 has a finite thickness. The foil is a dense medium and thus
o 8
absorbs a large amount of the fission energy available. Calculations
should therefore include this second medium unless the fuel is in a
gaseous form, such as UF^. It is very tempting to assume that only
perhaps one-half of the energy available v/ill get through the foil
into the gas. This assumption would be hard to prove because of the
difficulty of relating a measurement of this energy in one particular
experiment to a calculation where either the thickness or the density
of the uranium compound is different.
To calculate energy deposition at any point z of Figure 2.1,
one first assumes that scattering of the fission fragment by the medium
is negligible and that only straight line paths need be considered.
The origin of the geometry is at the left face of the source slab which
has a thickness R^, the range of a fission fragment in the source medium.
When x is larger than the substitution z.- x R^ is made so that
z = 0 at the interface. The source is assumed isotropic in emission
with azimuthal symmetry about x. The angle between the path and the
x-axis is 0 The slowing down of the particle in both media is
described by equation (4). While the fragment is in medium I moving along
the abscissa, the residual velocity at x v (x^x), of a particle borne
at x with initial velocity v^ is
v1(x';x) = v kJx' -x| x < x' < (9)
while for medium II
v2(z;x) = C(x) K2z ,
(10)


Figure 2-1 Geometry


22
where C(x) is the residual velocity at z 0 or the interface of a
particle born at x in medium I. Assuming continuity at the interface,
V* ;X>|x'=E1 = V2(Z;X)|Z=0
then
C(x)
Vi K1(R1 X)
(ID
and thus, the residual velocity in medium II is
v2(z;x) = v K^R x) K£z
(12)
Since the thickness of medium I is equal to the range of a
fragment in medium I, equation (11) is valid for any 0 < x < R^.
For a fission fragment not moving along the abscissa, but in the
direction 8 = cos ^p,equation (12) becomes
(R1_X) z
v2(z;il,x) = V. Kx K2 ,
(13)
provided that
(Rl-x) z
K, + K0 < v for all p, > 0
1 p 2 p o
or, in other words, provided that the particle arrives in medium II.
Since it was previously shown in equation (5) that
one can state that


23
r r1-x z
v2(z;1i.,x) = V1 -¡l-J .
(14)
The Energy Transfer Function of equation (8) can now be stated as the
two-medium function
1 2
F(z;|i,x) = M1v2(z;|jx)
r (Ri~x) z ~|2
Ei L M^2-J
(15)
In order to eliminate the dependence on a conversion factor a is
derived from the Bragg-Kleeman rule which converts the range of a
charged particle in one medium to its range in another medium.
Therefore,
and
where
and
r2 = r2 (VV1/2 Ri
R2 = aRl
a = (A /A )'1/2
P2 2 1
(16)
(17)
p = density,
A = atomic weight.
"a" may also be derived from the theoretical stopping equation
or from experimental measurements. Equation (14) thus becomes
r (R-.-x) ~i ~
G(z;|i,x) = E 1 %\ (18)


24
From the general geometry of Figure 2-1, a total energy current
is derived for a point r in medium II due to the source S(ro,Eo>Q) in
medium I.
Vr>=/ drQ f f dE0S(roEo G(r'>r0>E0&
I o E
Q o
(19)
where
r = a spacial point in medium I,
o
"4
r = a spacial point in medium II,
Q = a solid angle characterizing the direc
tional distribution of the source,
E = initial energy of the fission fragment.
S(r ,E ,Q)dr dE dfi
o o o o
= the distribution of the fission fragment
source at r in dr at fi in dfi and
o o
at E in dE (usually a constant).
o o
G(r;ro,Eo,Q) = the energy at r, carried by a fragment

originated at r moving in direction 0
with initial energy E assuming no
scattering.
If it is assumed that C(x) is the fission density,
C(x) = Zf(x)9(x), and that f(EQ) is the normalized fission fragment
spectrum, then with isotropic emission, the differential source within
a thin layer dx at x, emitted in the solid angle width dpdcp with
initial energy E in dE is
o o
C
S(x,E ,p,cp)dx dE dudcp = f (E )dx dE d^dcp .
o o 4tt o o
(20)


25
Using the energy transfer function of equation (18) and equation (20)
in (19), one obtains the total energy current at z in medium II,
J (z), resulting from a distributed source of fission fragments in
E
medium I
Vz)
_1_
4tt
2rr
dE f(E )E
o o o
o
R1
*
dx
'/a
dp£(x)
aR^-ax+2
aR~
X
(^-x)
- )
aR )
(21)
Nguyen [38] discusses the limits of integration and how one
would analytically integrate this function. With a constant fission
density of C
CE R
P
VZ) = 2
1 Ti ^ 1 .2 2 1.3 3 2 2 .1
bz + b z +^bz -bz Bn (bz) J
energy
2 1
cm -sec
(22)
where
b =
1 _1_
aRl R2
R and R being the ranges of fission fragments in mediums I and II,
1 *-<
respectively, of a fragment having the initial energy E^. The required
boundary condition J,,(z)| =0 (or at bz = 1) is satisfied.
E U2
Equation (22) represents the total residual energy at point z.
The instantaneous energy loss per volume as a function of z is obtained
by taking the derivative of J^iz) with respect to z.
E


26
Vz)
dz
CE R
P
10
. 3 2
b z
- 2b2z
B/n (bz)
-]
energy
3
cm -sec
(23)
An almost identical empirical energy deposition relationship can be
derived, as previously noted, based upon the relationship
E(x) = E
i 2
R
n
1 < n < 3 .
(24)
Both equations give similar results for small z, but vary considerably
for z approaching the range Rin medium II.
This energy deposition function ignores any nuclear elastic
collisions; but if one calculates an ion production source, a so-called
"ionization defect" takes into account this nuclear deposition, which
is less effective in ionization than coulombic interactions.
At this point researchers split to several different techniques
for generating source terms for a kinetic system. Most studies have
constructed an ion source term and used the standard w values for
fission fragment interaction with various gases. These values include
the "ionization defect" and are experimental in origin.
Using the square law point deposition form of equation (23),
one can derive, simply by dividing by w, the volumetric ion production
rate.
I.
i
1
dJ (z)
E
w. dz
i
CE .R
Pi
2w
i
Aiiv
n. L i
2 2 2
z 2b. z Qm. b. z
i i
ion pairs
3
cm -sec
(25)
where the distinction is made between the light and heavy groups of
fission fragments. Therefore,
V2> \ Vz) I Vz>
(26)


27
The assumption that w is a constant value over the
ion pair
entire path of the fragment is false, but if one includes the "ioniza
tion defect and views the target as a whole, such as a plasma system,
this approximation should be close to the actual generation rate.
P. Thiess [17] approached the problem in an unusual manner. Using
the semiempirical energy deposition approach, a suggested alternative
shown above, he avoids the use of w values by calculating excited states
and inoization directly. This approach requires knowledge of a complete
set of cross sections for generating the source terms for excited levels.
Thiess used modified Bethe-Born cross section data based upon proton
impact. Russell [16] used another approximation, the Gryzinski electron
interaction cross section, for his excited state calculations. Both
authors clearly state that the use of these cross sections may be
entirely invalid, but must be used because there are no experimentally
measured cross section data available for such interactions. One factor
that may make the Gryzinski electron interaction approximation more
applicable than the others is the fact that about two-thirds of the
ionization and excitation is distributed to the gas by secondary delta
rays or fast electrons, rather than by the primary fission fragment
particle.
The range of a fission fragment in a gas is a function of the
density of that gas and its molecular weight. Range relations are
strictly empirical and are derived from measured data independent of
straggling or other statistical phenomena.


28
Range as a function of pressure can be calculated using the
following equation [41]
R(cm)
where K = 1.4 for most gases (Figure 3-5).
Figure 2-2 shows a plot of range vs. pressure for both the
light group (E = 98.7 MeV) and heavy group (Eo = 67.5 MeV) fission
fragments in argon and helium.
Experimental procedures such as those used in this dissertation
are based on cylindrical geometry. The average chord length
(s ss 4 volume/area) best represents the distance that a particleif born
on the surface or in the volume of the cylinderwould travel in a
straight line before it would collide with the surface. For a cylinder
30.5 cm in length and 3.7 cm in diameter, the average chord length
is 3.4 cm. These lengths are identical to those found in the experi
mental apparatus used here. It is interesting to note in Figure 2-2
that at all pressures below 1 atmosphere (760 torr), the range of
fission fragments in helium is greater than the average chord length.
The situation for argon is different since it is ten times as dense for
equal pressures; therefore, the average chord length is equal to the
range of the light fragment at 360 torr and equal to the range of the
heavy fragment at 280 torr. A quick conclusion could be that for most
of the experimental data that one would observe, only a small fraction
of the fission fragment energy would be deposited in the gas. This is
not necessarily true, because the energy deposition from the foil is


RANGE (cm)
29
Figure 2-2 Range of Fission Fragments
in Helium and Argon


30
skewed towards the foil surface due to the finite thickness of the
source and the fact that the great majority of the fission fragments
do not leave the source surface with the typical 67.5 MeV or 98.7 MeV
average energies that they are born with.
A much better view of the energy deposition can be gained by
calculating the deposition profile at each pressure. A calculation
of the energy deposition utilizes the square law deposition function
and geometry used for equation (23). First, several assumptions must
be made in order to equate the slab geometry calculation to the cylin
drical geometry that is presented in most experimental situations.
1. The slab and cylindrical two-region energy current functions
are essentially identical.
This is a good approximation since the range of a fission frag
ment in the U0 source foil used in these calculations is only
O O
-4
7.5 x 10 cm; therefore, the great majority of the energetic fission
fragments that have a considerable range are emitted perpendicularly
from the surface.
2. Little energy is emitted to the gas when a fission fragment
collides with a surface.
This assumption is not adequate for exact analysis but should
be valid for the accuracy required here.
3. Energy deposition by other sources is a very small fraction
of the fission fragment deposition.
This assumption has been proved experimentally to be valid
by Leffert [26] where he has shown that other sources, such as gamma


31
radiation, deposit less than 1 per cent of the total energy to a volume
in normal reactor situations.
In order to proceed further, the fission rate must be calcu
lated as follows:
C = Rf = N a § = E $
(27)
N = number density of target nuclei
CT = fission cross section
§ = average neutron flux along the foil
E = macroscopic cross section.
For these conditions,
2
Thickness =6.2 mg/cm (the range of a fission
fragment in U 0 )
J O
Average thermal flux = 3.8 x 10^
cm -sec
Fission cross section = 505 barns 93% enriched uranium
the generating function per cm surface area is 8.06 x 10
11 fissions
2
cm -sec
From equation (23)
i=l,2
(28)


32
where
E
P
b
i
fission rate
most probable energy at birth
R
aR_
2i "li
fission fragment group.
(each group)
This generating formula is calculated by splitting the depend
ence on light and heavy particles, then adding the results, giving the
energy deposition profile shown in Figure 2-3 for helium and Figure 2-4
for argon.
The gas pressure, or atom number density, is the most important
factor in the deposition of energy in a fixed cavity. For pressures
below 760 torr in helium, the energy deposition across a 3.4 cm average
chord length cavity is approximately uniform. But, in argon, only
below 75 torr is the energy deposition somewhat uniform across the
cavity. Since this calculation takes into account only coulombic inter
actions and ignores the nuclear elastic and inelastic scattering of the
particles when they reach the neutral status, the energy deposition
curves fall off extremely fast. If the nuclear scattering terms were
included, the range would be extended slightly, but only a small addi
tion would be made to the deposition of energy at the end point of the
fission fragment path. The effect on the total deposition would also
be small [37],
One of the unknowns, as previously described, involves how the
energy is utilized, what excited states or ions are produced, and what


DEPOSITED ENERGY (MeV/cm -sec)
33
10 101 102 103
DISTANCE FROM U308 FOIL, Z (cm)
Figure 2-3 Deposition of Energy into Helium
by Fission Fragments, $ = 3.8x10^ 2
cm^-sec


DEPOSITED ENERGY (MeV/cm -sec)
34
DISTANCE FROM l^Og FOIL, Z (cm)
Figure 2-4
Deposition of Energy into Argon ^
by Fission Fragments, $ = 3.8x10
cmz-sec


35
photon emissions are coming from the "plasma." These items are
a function of cross section for the various species that are present
in the gas. Measurements of the photon emission of the gas are based
on total emission from the optical cavity; thus, this photon output
can be compared to the total energy deposited into the gas in this
cavity. A description of the total energy input can be obtained by
integrating the energy deposition function over all source areas and
over the average chord length. From equation (23),
E =
dA
dJE(z)
dz
dz
A CE R o o 9
E = j lb z 2b z V/n (bz)
-]
dz ,
where
z = average chord length, or
z = R2, if R2 < z
i = R = range of fission fragments in gas and is
b 2
a function of pressure.
Integrating,
z
MeV
sec
o
E =
/i n
f P
b z 2 2
b z (fa bz
Â¥
bz^J
(29)
(30)
(31)
Again, as in equation (28), the calculation is split for each
group of fission fragments. Figure 2-5 shows the solution of equa
tion (31), where E is calculated as a function of the gas pressure for


ENERGY DEPOSITION (MeV/sec)
36
101 102 103
PRESSURE (torr)
Figure 2-5 Energy Deposition by Fission
Fragments in Argon and Helium
- A Fixed Cavity -


37
the representative cylinder with an average chord length of 3.4 cm.
The deposition in the cavity filled with helium is almost a linear
function of pressure. In argon, the effect of the range being less
than the cavity dimensions is evident by the leveling off of the curve
above 200 torr. Depending on the recombination and diffusion of elec
trons at pressures above 200 torr, the fission fragment-produced
excitation may generate a torroidal luminescent output in the cylin
drical cavity. This would alter the uniformity of the photon output
into the fixed solid angle view of the diagnostic equipment and may
provide erroneous data, especially if some of the surface region were
optically shielded from the detector system. It is estimated that such
a shading effect exists in the experimental equipment associated with
this work. Further review of this problem can be found in Chapter 4.
3
2.2 Energy Deposition by the Reaction He (n,p)T
in a Glow Discharge
3
High energy products of the reaction He (n,p)T are of interest
3
here because of the use of He in the glow discharge experiments to be
described later.
The proton and triton share the reaction energy of 760 keV with
the heavier triton taking 190 keV and the proton 570 keV. The initiat
ing neutron energy is in the range of less than a few eV; therefore,
little momentum is transferred and the reaction particles travel
randomly in opposite directions. Thus, the interactions with the gas
are independent of one another.


38
Fortunately, the linear stopping power formulation for protons
and heavy-heavy protons (tritons) has been established as satisfactory
for calculating energy loss phenomena. Interesting calculations for
this reaction include total energy deposited in the cylindrical glow
discharge and total ionization produced by this deposition. These
3
calculations are done assuming that the gas is He at a pressure of
dE
15 torr for an 8:1:1 mixture of He-CO -N is 2.6 times that of
dx 2 2
helium [13]; therefore, the calculation of total energy deposited
should be multiplied by this amount for experiments involving C02 gas
mixtures. Reference 8 gives the stopping power of helium as
dE
^ = 105
dx
eV
for
570
keV
protons,
cm-torr
dE^
T
970
eV
for
190
keV
tritons.
dx
cm-torr
For a cylindrical cavity 3.7 cm in diameter and 12.7 cm long
(identical to the dimensions of the experimental apparatus) the average
chord length is 2.87 cm.
The total energy deposition is calculated using the following
equations:
1. Reaction rate
_3
R = N^ct$ cm (32)
3
where N = number density of He atoms
c = thermal neutron cross section = 5400 b
11 2
$ = thermal neutron flux 3.8 X 10 n/cm -sec.


39
where
P
V
Total energy deposition
p T
= average chord = 2.87 cm
= pressure = 15 torr
3
= volume = 136 cm .
(33)
3. Total energy available
keV
E = (760 keV) RV
sec
(34)
Upon application of the data to these equations, it is found
13 eV
that only 1.75 x 10 is being deposited into the cavity. This is
14 eV
only one-tenth of the total available energy, 1.12 x 10 generated
-6
in the cylindrical volume.
This energy input is equal to only 2.8 x 10 watts, so the
total energy both available and deposited at this neutron flux level
is but a small fraction of the energy deposited by electrical excitation.
In fact, measurements that will be detailed in Chapter 4 for glow dis
charges show that the minimum electrical power input needed to generate
a glow discharge in such a cavity is 0.5 watt. The one conclusion that
can be drawn from the calculations is that volume ionization or excita-
3
tion by He reaction products probably does not account for any signif
icant changes in the operation of typical low power glow discharges,
12 2
especially for neutron fluxes below 10 n/cm -sec.
Butler and Buckingham [42] state that for high energy ions
whose velocity is much greater than the thermal ion or electron


40
velocity, the loss rate of energy to the electrons is larger than to
2 3
ions by the factor (m./m )(p /z. p.). For He this ratio is approx-
i 0 e i i
imately 20. This could account for some volume enhancement of energy,
especially in the case of fission fragment deposition. But, and
p. are extremely small in both cases and most of the energy transfer
is to neutral particles. This effect then, is not significant in the
tenuous plasmas described here. Since it has been established [11,13]
that the nuclear reactor does affect the operation of a glow discharge
and thus laser operation, the changes occurring must be a function of
either changes in glow discharge structure or irradiation of the elec
trodes. Data describing these effects are presented in Chapter 4.
2.3 Description of a Fission Fragment-
Produced Plasma
At present much effort is being expended in the area of char
acterization of the tenuous "plasma" produced by fission fragment
sources [ 1 ]. The assembly of a set of kinetic rate equations is the
ideal approach to the characterization of this gas. But, because of
this method's detailed description of the number density of all species
and their important excited states, all reaction cross sections must
be known. Considering the number of species of a gas (atoms, ions, and
molecular combinations) and the excited states possibly present in
these species, this becomes an arduous task.
In most experimental processes, a small amount of impurity
gases are always present. These impurities enter into the kinetics of
the system and complicate the rate equation approach even more.


41
An example of this is the presence of a small amount of nitrogen.
Even in amounts of less than one part per million, spectroscopic anal
ysis of an alpha particle or fission fragment excited gas show the
presence of the first negative system of N+ with very intense band
z
peaks. This indicates the presence of an additional ion generating
term of significant magnitude to alter the population of many species.
N* is formed in several ways. The two most important transfer reac-
z
tions are
Hemetastable +
N
He +
N2 +
e + AE
and
He2 +
N
2He +
N2 +
AE
(35)
(36)
The Penning type ionization specified in reaction (35) is
normally considered the predominant reaction for the formulation of
the N+ ions. Thus the population of is predominately a function
3
of the population of the metastable He(2 s) state and the recombina
tion rate of N*. N+ will then increase as a function of increased
Z Z
helium gas pressure, since the collision rate, as well as the meta
stable population, also increases as a function of pressure. The reac
tion described in equation (36) also produces the N* ion, but at a
rate about five times slower than the Penning type ionization rate [43],
This is still significant, but the effect is diminished even more
because the population density of the molecular ion is far less than
the metastable state density.
The molecular helium ions are formed in many ways. The follow
ing reactions generate the majority of the ions.


42
He+ + 2He He* + He (37)
o O
He(2 s) + He(2 s) He* (38)
More information on formation and decay of these molecules is given
in References 43, 44, 45 and 46.
If the excited states are neglected and only number densities
of ion, atomic, and molecular species are included in the rate equa
tions, the set of equations is reasonable and easily solved with the
inclusion of only a few unknown reaction cross sections. Examples of
this technique, which include the effects of wall losses from the
excited gas, are given in References 26 and 47.
In order to study fission fragment-produced excitation without
using rate equations, it is advantageous to assume some model. Such
models, although probably invalid for exact representations, should
use an equilibrium distribution of excited states based on Maxwell-
Boltzmann statistics or some combination of equilibrium distribution,
plus a calculation of individual excited states by approximate cross
section.
The latter approach was used by Russell [16] in his calculations
of population inversions in argon. This model is presented here since
it is reasonably complete and takes into account most of the processes
for forming excited states in an individual manner, rather than by
empirical statistical distribution methods. It does ignore all
excited states other than those of atomic argon, and it would require
extensive modification to include analysis of ion excited states which
are experimentally available for study in fission fragment-generated


43
plasmas. Also, no provisions are made for inclusion of impurity species
in the equation set, but they could be added without great difficulty,
since most impurity interactions are loss terms for the primary gas.
This semiequilibrium model is similar in many ways to that used
by Leffert [47], except that in the latter case no attempt was made to
calculate excited states densities.
Using the theory of Bates, Kingston, and McWhirter [48],
the production terms for argon excitation have been reduced to five
principal processes:
1. Recombination of thermal electrons with atomic ions
2. Inelastic collisions between excited atoms and thermal
electrons
3. Radiative transitions
4. Direct excitation due to fission fragments and high
energy secondary electrons
5. Formation of excited states in the products of dissocia-
- *
tive recombination of diatomic ions (He + e -* He + He ).
Combining the above processes, an infinite set of excited
state density functions are obtained.
CO
CO
qp
q co
+ n
e
qp
q>p
+ S.
(39)


44
where
n . =
(P)
n =
e
n. =
(q)
K, ,
(P,c) =
K . =
(p,q)
A(p,q)
G(p,q)
K(q,p)
A(q,p)
G(q.p)
K(c,p)
excited state number density, state p
electron number density
excited state number density, state q
inelastic cross section for collision of an excited
state with a thermal electron producing ionization
(loss term)
inelastic cross section for collision of an excited
state with an electron producing excitation from
p to q (loss term)
radiative transition rate for loss by a transition
from excited state p into q
correction term to account for optical trapping in
resonant transitions, transition from p to q
inelastic cross section for collision of a thermal
electron with the excited state q producing the
excited state p (gain)
radiative transition rate for gain by a transition
from excited state q into p
correction term to account for optical trapping in
resonant transitions, transition from q to p
cross section for 3-body recombination from continuum
to excited state p (gain)
radiative recombination cross section producing
excited state p (gain)


45
= source term for formation of excited states in the
process of dissociative recombination (gain, but
usually ignored).
S$ n T]* is a production term for excited states (p) due
a (p)
to direct excitation from fission fragments and the secondary electrons
they produce. This term is assumed constant throughout the volume in
question and is analogous to the production rate for atomic ions.
Sin = partial generation function that includes neutron
a
flux §, atomic number density n and a geometry
cl
term S
T] = ratio of total excitation rate to atomic ion produc
tion rate = 0.53 [24]
\lr = ratio of the excitation cross section for array p
(P)
normalized with the cross section for the first
excited state (i.e., for argon, the 4s array),
assuming
I
n=2
(P)
= 1.0
(40)
The cross section ratios can be calculated using the theory of
Gryzinski [49] for electron-atom interaction or by any other method.
If relative excitation cross sections were known from experimental
measurements, they also could be inserted at this point.
The argon ion density can be.represented as follows:


46
^ = S n mn^ Ar+ D
dt a a 1 .2
n A
a
ne I fne [K(c,p) + 9(p)l n
P=1 ^
.K
(P) (P,c) (
(41)
where
S$n = direct ionization source term from fission fragments
a
and secondary electrons
2 +
-mn Ar
a
= loss term by generation of the molecular ion Ar^
Ar
-D = loss by diffusion from the volume of interest.
1 >2
n A
a
The next three terms are, as described previously, loss by
3-body recombination, radiative recombination,
The molecular ion density equilibrium is
dAr
dt
2 A +
mn Ar
a
Ar,
tv Ar n
D 2 e
- D,
2 a2
n A
a
(42)
where
2 +
mn Ar = 3-body collisional production term
-o Ar n = recombination loss term
D 2 e
Ar:
-D
2 a2
n A
a
= diffusion loss term.
The electron balance is
n = Ar+ + Ar^ ,
e z
(43)


47
d( n kT ) m
2 e e e
= 4 kn
dt me
a
8kT
(n q + n q ) (T -T )
nm e ei a ea e a
+ + sKEqd
rec rad a Se
(44)
The first term on the right-hand side is the elastic collision energy
loss assuming a Maxwellian distribution of electron energy about the
electron temperature T .
e
q = electron ion cross section
ei
q = electron atom cross section
ea
Q = gain in thermal electron energy from inelastic
rec
electron atom collisions
Q = line and continuum radiation losses
rad
S$n E = energy source term from fission fragment interactions,
a Se
The time dependence of all the rate and equilibrium equations
presented is much faster than any change in the fission fragment source
term; therefore, steady state solutions can be obtained by setting the
time rate of change of Ar+, Art, n T and n. to zero.
2 e e (p)
Equations (39), (41), (42), (43), and (44) are an infinite set;
in order to generate a solution an approximation is required. Since
there exists a level adjacent to the continuum that is in Saha equilib
rium. at the electron temperature, it can be assumed that all levels
above this are populated with a normal Maxwell-Boltzmann statistical
distribution of states. If the n, set of equations is truncated at
(P)
this p level, a closed set is obtained. The obvious problem is what
level to truncate the excited stat population calculation. Russell


48
assumed equilibrium above the 6p level and solved a set of thirteen
simultaneous equations by computer methods. His solutions for Ar I
indicate the presence of inversions in the 5S-4p and 4d-5p transitions.
Although the capability of lasing these transitions has not been
determined, other transitions of Ar I have been made to lase.
In review, this chapter has shown how a fission fragment
deposits energy and how one could calculate this deposition in several
3
geometries. It has been shown that the He (n,p)T reaction products do
not deposit significant amounts of energy into the volume of a glow
3
discharge in 15 torr He A model of the reaction kinetics of a fis
sion fragment-generated "plasma" has been presented in order to
describe the basic processes that occur in such an excited gas.


CHAPTER 3
PLASMA RESEARCH APPARATUS
3.1 Introduction
Since previous researchers [33,35] have been fraught with great
difficulties when attempting spectroscopic analysis of in-reactor
plasmas, it was imperative that certain basic design criteria, devel
oped as a result of this previous work, be applied to the construc
tion of this apparatus.
Most of the difficulties involved the transmission of the
spectrograph of the low level light produced by the fission fragment
plasma. The glow discharge experiments have adequate light output to
overcome these problems; therefore, design was optimized for the fis
sion fragment interaction experiments. The experimental chamber and
peripheral equipment were developed using the following criteria:
1. Chamber size must be large enough in average path length
to take full advantage of the energy available from the
average fission fragment.
235
2. U fissionable coatings should be maximized in area and
thicker than the mean free path of a fission fragment in
the coating.
3. Solid angle light availability to the optical system from
the plasma should be optimized.
49


50
4. Luminescent components such as quartz (light pipe) should
be eliminated from the optical path where subjected to
large neutron fluxes.
5. The experimental chamber should be located at the highest
flux position available in the reactor and should contain
only low thermal neutron cross section material (except
235
for TJ in the fission fragment plasma experiment).
6. A high light power spectrograph and extremely sensitive
photomultiplier -should be used instead of photographic
techniques.
7. The design should include the capability of using high
purity gases.
The above guidelines were followed, utilizing trade-offs where
necessary, and the resulting apparatus, as described in this chapter,
proved quite successful in providing excellent spectral data.
A detailed set of criteria for generating data of the quality needed
to determine cross sections is available in Reference 32.
3.2 Primary System
Several alternate methods of studying spectroscopically an
in-core plasmawere investigated and two basic solutions were identi
fied: (1) a small spectrograph installed next to the plasma, internal
to the reactor, providing a large solid angle light gathering capabil
ity, and (2) the optical transmission of light up a tube to a spectro
graph.


51
The second method was chosen as most practical. It employed
a stainless steel vacuum chamber 9 feet in length and 7/8 inch in
diameter, with a standard Ultek cross on top (Figures 3-1,3-2), where
the light is transmitted at right angles to the vertically positioned
spectrograph. Various experiments were inserted into the tube where
they were held at the bottom by gravity.
Emphasis was placed on the use of standard fittings, flanges,
and sizes. This allowed the replacement and storage of activated
9-foot tube sections, thereby allowing experimental procedures to con
tinue without waiting for an activated section to decay.
3.2.1 Plasma Region
The outer stainless steel vacuum jacket allows insertion of
both the glow discharge and fission fragment apparatus into the high
neutron flux region of the reactor. The glow discharge experiments
included study of three different types of cathodes, flat, brush, and
hollow. The insulating structures for the flat and brush cathodes
(Figure 3-3) consisted of an outer 2 feet by 40-mm O.D. Vycor tube
with the bottom beveled inward. The cathodes made continuity with the
outer shell by gravity contact on the bottom of the casing. The ring
anode was spaced from the cathode by a 35 mm by 5-inch Vycor tube.
Electrical connection to the anode was made by an insulated wire run
ning up the inside of the tube.
The hollow cathode structure was similar except a Vycor insert
was built to support the small cathode.


52
Figure 3-1 Reactor Mounting


53
GLOW DISCHARGE EXPERIMENT
FISSION FRAGMENT EXPERIMENT
Figure 3-2
Chamber Experimental Sections


RING
za udi
.. t
:
/
/////////A
BRUSH AND FLAT CATHODE
GLOW DISCHARGE
HOLLOW CATHODE GLOW
DISCHARGE
FISSION FRAGMENT
EXCITATION
Figure 3-3 Chamber Detail Reactor Region
30.5 cm


55
Removal of these structures to allow insertion of the next
assembly was a simple matter of turning the chamber upside down, and
sliding out the apparatus.
The fission fragment interaction assembly (P'igure 3-3) was
a 40 mm diameter, 3-foot-long Vycor tube with a 30.5 cm length inter-
235
nal coating of U 0 and an indentation at the 30.5 cm distance to
O O
support the anode. For comparison, a glow discharge was occasionally
started inside this assembly, using the vacuum chamber bottom as
a cathode.
3.2.2 Vacuum Chamber; Optical, Gas
and Electrical Feeds
All chamber parts were designed around "Ultek" 2-inch
flanged fittings in order to aid in replacement and modification.
The outer shell (Figure 3-1) consists of a 9-foot, 1-7/8 inch O.D.
by 0.065 inch thick No. 304 stainless steel tube with a heliarc-
welded plug on one end a standard 2-inch fitting heliarc-welded on
the other end.
Placed vertically on top of the long tube is the 2-inch
standard cross. Matched to the cross is electrical feed through on
one side for connection to the anode, gas feed on the top and a vinyl
sealed quartz window on the other side.
The optical system consists of a 500-mm focal length fused
quartz plano-convex lens held and focused vertically by three align
ment wires (Figure 3-1). A right angle front surface mirror is held
and aligned by a mount inserted into the center of the cross. The
vinyl seal quartz window allows light to escape from the chamber and


GRAPHITE SIACKINS (3) IWWK1EI wtsxjt
CJi
a
Figure 3-4 University of Florida Training Reactor


57
be focused 2 feet to the side on the entrance slit of the spectrograph.
Thus, the plasma is viewed through the ring anode at a solid angle
-4
of 1.18 10 steradians, and focused by the lens on the spectro
graph entrance slit after passage through the exit window.
-6
The maximum vacuum attained by the system was 1 X 10 torr
and the maximum design pressure was 760 torr.
3.3 Uranium Coatings
3.3.1 Coating Requirements
One of the most important factors in the production of
a fission fragment interaction plasma is the fabrication of a suitable
uranium coating for the experimental chamber. Requirements for the
coating included the capability of deposition on the interior of a var
iety of cylindrical surfaces, such as Vycor and stainless steel.
Interior dimensions from 10 mm to 44 mm and lengths up to 3 feet were
encountered.
3.3.2 Coating Thickness
In order to maximize the source strength and thus the
number of fission fragments available, coatings were made thicker than
the range of a fission fragment in the source material. The range of
a fission fragment passing through U^Og, the final product of the
coating procedure, is calculated [41] as follows, with K and E from
Figures 3-5 and 3-6:
cm
(45)


58
O 5 10 15 20
DENSITY (g/cm3)
Figure 3-5 K as a Function of Density


KINETIC ENERGY OF PRODUCTS (MeV)
59
MASS NUMBER A
Figure 3-6 The Kinetic Energy of Fission Fragments as
a Function of Mass Number r38]


60
Density of U 0 =8.3 ^
O O
cm
K for U0o = 0.294
O
mg
(cm2) (Me\f/3
Maximum expected fission fragment kinetic energy = 97 MeV,
for mass = 95; therefore,
mg
R = 6.206
cm
2
mg
A coating thickness of 10 = was considered adequate to
cm
account for some nonuniformity of application.
3.3.3 Review of Methods and Chemistry
There are several methods for producing coatings including
ion deposition, electroplating, powder distribution on a binder, and
coating and ignition.
For the purposes of the fission fragment interaction exper
imental work the most flexible and inexpensive technique, coating and
ignition, was chosen.
Much detailed work was done in this area at Los Alamos Scien
tific Laboratory around 1945 under the title of "Zapon Spreading
Techniques" [ 51].
The basic principle [52] of the Zapon spreading technique is
as follows: An alcoholic solution of the nitrate of the substance to
be deposited is mized with a dilute solution of Zapon lacquer in alco
hol, acetone, or Zapon thinner. The resulting solution is spread or
painted on the foil backing, allowed to dry, and then ignited to remove
organic substances and to convert the nitrate to oxide.


61
Many variations of this technique are possible, and it is
applicable to a wide variety of substances. The procedures used in
this project generally follow those suggested by this work.
Many alternate methods of placing coatings on surfaces were
evaluated, but the only successful results were obtained when many
thin coatings -were added in succession.
The requirements for a successful coat include a liquid that
can be deposited in thin layers, does not evaporate too quickly, and
includes a binder to transfer the fluid to a very viscous substance
upon evaporation of the solvents. The binder is necessary to prevent
an unequal distribution on the surface.
The Zapon spreading technique for uranium used ethyl alcohol
235
as a solvent for U 2^N3^2 6H20 and added Zapon lacquer as a
binder for the uranyl nitrate salt upon evaporation of the ethyl
aleo hoi.
Zapon lacquer is not available, so a chemical substitution of
"Testors" butyrate dope containing methyl cellosolve and isobutyl
alcohol was used. Unfortunately, this lacquer forms a gel with ethyl
alcohol so n-butyl acetate was added to dissolve the lacquer.
235
A detailed description of the preparation, of uranium foils is
given below.
3.3.4 Chemical Procedures
The procedure for producing the coating solution, as
detailed in Figure 3-7, is variable depending upon the form of metal
available. The following procedure starts with highly enriched
uranium (93%) metal.


Figure 3-7 Chemical Procedures
Coating Solution
o
to


63
1. Dissolve the metal in concentrated nitric acid (HNO^).
2. Dry the solution on a hot plate with the temperature below
200F in order to avoid hot spots and thus production of
any UO The result is UO [NO ] 6H 0, a bright yellow
powder.
235
3. For each 4 grams of U add 20 ml ethyl alcohol, 20 ml
of butyl acetate, and 20 drops of butyrate dope.
4. Variations in the above mixtures are possible, but the pro
portions given seem to work well in the coating process.
3.3.5 Mechanical Coating Procedure
The art of producing a U 0 coating involves application of
O o
many thin coats in order to avoid flaking of material. The following
procedure is detailed in Figure 3-8.
1. a. Vycor base Using a clean tube, flush with 6NaOH
and then with distilled water,
b. Metal base Using a clean tube, flush with 6N HNO^
and then with distilled water.
2. Place the cylinder on a rotating horizontal mount.
3. While the cylinder is rotating, place a thin, even coat
of solution on the inside of the tube, using a coating
tool such as a camels hair brush or, for long tubes,
a tube swab mounted on a wooden dowel.
4. While the cylinder is rotating, dry the coating with air.


Figure 3-8 Mechanical Procedures
for Coating
O


65
5. Fire the coating using a Fischer burner or propane torch.
This will first oxidize the uranyl nitrate to brown-colored
UO and then at higher temperatures to black-colored U 0 .
2 3 8
The butyrate dope will evaporate and leave a residue of
less than 1 per cent.
2
6. Repeat until coating thickness is at least 10 mg/cm .
Forty coats were adequate for the Vycor substrate.
The resultant coatings appear as a black ceramic material with
a surface area much greater than that of a flat substrate. This is
due to the porosity of the ceramic coat and has likely aided greatly
in the deposition of larger amounts of fission fragment energy into
the surrounding gas.
235
Since U is radioactive and most samples contain traces of
other isotopes, care was taken to properly handle and contain the
chemicals involved in the coating procedure.
3.4 Support Systems
Acquisition of various data describing the effects occurring
in a plasma is dependent on the following support systems.
3.4.1 Reactor: Neutron Flux and Gamma Dose
The experimental chamber was designed to be inserted into
the University of Florida Training Reactor. As shown in Figure 3-4,
the UFTR is an Argonaut-type reactor licensed to operate at 100 kW.
The thermal neutron flux available.in this facility at 100 kW is shown
in Figure 3-9 as a function of distance from the bottom of the


66
o
CD
LO
I
X
ZD
O
Figure 3-9
Distribution of Thermal Neutron Flux
along Experimental Chamber


67
experimental chamber. These measurements were taken, using standard
gold foil dosimetry. In order to measure the thermal neutron flux
actually available to the plasma region, all foil irradiations were
done inside the stainless steel experimental chamber. At 100 kW the
11 2
average flux over the length of the glow discharge is 4.7 x10 n/cm -
11 2
sec, and, over'the fission fragment plasma, 3.8 x 10 n/cm -sec.
7
Gamma dose in this area at 100 kW is estimated to be 1.1 x10 R/hr
at equilibrium.
Reactor power data relate directly to the flux and are based
upon two calibrated compensated ion chambers placed near the core.
The experimental apparatus was placed in the 1-7/8 inch center verti
cal access port located between the two fuel regions. This is the
highest thermal flux region available in the reactor, but it is also
the highest reactivity worth region. This presented certain problems
which will be discussed in Section 3.4.5.
3.4.2 Electrical Systems
There are two systems involved in operation of the apparatus,
other than those pow'er supplies and leads involved in diagnostic equip
ment .
In order to supply a high voltage DC field to the chamber
when studying fission fragment interaction light amplification, a 10 mA
5 kV calibrated DC supply was used. For current measurements, the
power supply was floated with respect to ground on a 100 ohm resistor
across which was placed a Keithly DC microvoltmeter.


68
Electrical systems for operating the glow discharge were more
sophisticated because an arc in the chamber could destroy the contin
uity of the experimental procedure by altering the cathode surface.
Therefore, a sensing circuit was designed to monitor the voltage across
the glow discharge. Upon sensing the large negative transient when
the glow discharge changes from an abnormal glow to an arc, Figure 3-10,
an extra resistive load is switched into the series load chain in order
to quench the arc and return the system to a glow discharge. Although
the quenching system operated effectively, it was rarely needed, as
will be explained in Chapter 4.
Glow discharge I-V data were obtained either by two voltmeters,
one connected to read glow discharge voltage and another across a 2 ohm
calibrated resistor to measure current, or by direct connections to an
x-y plotter.
The glow discharge electrical source consisted of three series-
connected ultra-stable Lambda power supplies with both variable volt
age and variable load controls. This system alloived operation over
wide ranges of gas pressure and glow regions.
All of this equipment was installed in racks and operated
remotely on the floor of the reactor cell, since dose levels were too
high on the reactor top face to allow long term access by personnel.
3.4.3 Gas Filling Systems
Two different systems were used for filling the chamber.
One of the systems, designed for ultra pure gas filling and mass anal
ysis of filled chambers [31], was located remotely from the reactor


Figure 310 General Gas Discharge IV Characteristic
CT5
to


70
building, and could only be used in the glow discharge experiments where
neutron activation of equipment was minimal. Its capabilities allowed
precision filling of gases with impurities of less than 1 part per
million, and bake-out of wall adhered impurities such as ^0. The min
imum chamber pressure that was reached during pumping and bakeout was
6
1 X 10 torr, assuring the absence of substantial leaks in the system.
For the fission fragment interaction experiments, where the
Uo0 foil is highly activated, gas fill was done while the apparatus
O O
was mounted in the reactor. The gas filling system used in this case
consisted of a remotely situated two-stage vacuum pump, needle valve
mixing equipment and pressure indicating systems. Minimum pump pres-
-3
sure on the system was 1 x 10 torr, thus allowing an impurity source
5
of air, with a 1 atm fill of pure gas, of less than 1 part per 10 .
It was expected that the main impurity would be N9 and that this would
show up in the spectrographic analysis.
Since the above facility was not capable of ultra pure filling,
it was decided that commercial grade gases would be adequate for these
early experiments. The analysis of the argon and helium that was used
5
did, in fact, show impurities, mostly Ng, of less than 1 part per 10 .
All experimental work was done with the chamber sealed due to
safety regulation as will be described in Section 3.4.5.
3.4.4 Shielding
Two main purposes were served when the elaborate shielding
cave system was built.


71
First, the dose available from the center vertical port without
shielding would not allow reactor operation much above 1 kW, two orders
of magnitude below needed flux levels. Second, the ultra sensitive
photomultiplier used in diagnostics is sensitive to gamma and without
shielding the DC level and subsequent noise is intolerable.
The shielding system is diagramed in Figure 3-1 and shown in
Figure 3-11. The cave around the center vertical port consists of
lead filler rings surrounded by steel and lead blocks. Borated poly
ethylene blocks were used to moderate and absorb either fast or thermal
neutron flux transmitted up the access port.
A secondary lead cave was constructed around the photomulti
plier tube and constituted the light tight mounting case for the photo
multiplier as well as a container for the immediate electronics required
for its operation.
With this shielding, the DC shift from gamma sources was 7.5 mV
at 100 kW reactor power with a measurable spectrum line height as small
as 2.5 mV. After processing the signal, a noise component of about
1.1 mV overlaps the data.
3.4.5 Safety
Experimental procedures that involve insertion of absorbers
and unclad fuel into a high worth region of a reactor must also include
many safety considerations.
The center vertical access port, where the experimental work
was done, is located, as shown in Figure 3-4, between two fuel regions
in a graphite moderator. This area is considered a high reactivity


72
Figure 3-11 Chamber Mounting and Shielding Cave


73
worth region because it couples the two fuel regions together. Any
thermal neutron absorber inserted into this region affects the reactor
criticality situation much more than this same absorber placed, for
instance, in the thermal column, where the reflection of neutrons back
into fuel is minimal. The experimental apparatus is not an extremely
heavy absorbed, but its negative reactivity effect on the core was
large enough so that in certain circumstances, where heavy absorber
gases were used and where the tube was inserted to a greater depth
than normal, the reactor could either not achieve criticality or could
not run at high power due to the negative temperature coefficient of
reactivity.
This problem could be overcome only by allowing removal of
enough reactor control blade (neutron absorber) so that the decreased
absorption would overcome the negative reactivity of the experiment.
Initial control blade removal levels were limited by the reac
tor subcommittee of the University of Florida Radiation Control Com
mittee to less than 0.6 per cent positive reactivity insertion. With
a positive reactivity insertion of greater than 0.6 per cent, the
reactor is in a prompt critical excursion or critical on prompt neutrons
only and thus in an uncontrollable highly dangerous situation (pos
sible destruction of the core). But, due to the large negative reac
tivity presented by the experimental apparatus that would counter
balance positive reactivity, the reactor subcommittee allowed removal
of the control blades to a position corresponding to greater than 0.6
per cent positive reactivity when the following requirements were met:


74
1. The apparatus is absolutely fixed and cannot move.
This requirement was satisfied by proper placement of the
massive weight of the shielding cave which could not be moved without
deliberate actions.
2. The gas fill is fixed in pressure, less than one atmo
sphere, and will not be changed while the reactor is
critical.
This requirement was satisfied by sealing the chamber before
each run and by placing a relief valve at the fill valve to keep pres
sures greater than one atmosphere from entering the chamber.
The fission fragment interaction assembly somewhat eased the
negative reactivity problem due to the coating's addition of about
4 grams of fuel to the high reactivity worth region.
After many hours of high power irradiation, the glow discharge
experiments had an activity which gave surface dose rates of about
400 mR/hr. This decreased to about 100 mR/hr in a few days and was
deemed not much of a problem, especially since there was no loose con
tamination. The fission fragment interaction assembly contained a
large area of unclad fuel (coating); when removed from the reactor, the
dose rates at the tube surface were about 100 R/hr. Therefore, remote
handling of the apparatus by the reactor overhead crane and long term
storage in the water shield tank (see Figure 3-4) was necessary before
disassembly of the chamber. The internal components of the chamber,
especially the upper section, were heavily contaminated with mixed fis
sion products and had to be handled properly during disassembly.


75
The vacuum pump exhaust which contained various radioactive
41 40
gases, usually Ar from activated Ar was connected to the
UFTR's air handling system for filtration, dillution, and disposal.
The problem of cooling the glow discharge was handled by the
same air handling system, which displaces about 12 CFM through the
center vertical port.
3.5 Data Acquisition Systems
I-V, reactor power, and spectroscopic data were taken during
experimental runs. Current and voltage measurement are an integral
part of the electrical supply system and were described in Section
3.4.2. Data on reactor power, and thus neutron flux, were obtained
from the reactor operating console, utilizing two compensated ion
chambers.
Spectroscopic data were obtained using a McPherson, 3/4 meter,
criss-cross, Czerny-Turner mount, scanning monochrometer with the
O
grating blazed for 3000 A and an EMI 9558 QB photomultiplier tube
mounted in the shield cave previously described. Since the lens does
not identically focus all wavelengths on the entrance slit, the system
was operated in a slightly defocused manner to allow for less precise
alignment of the optical system. The photomultiplier cathode was
operated at -1300 volts DC and its load was 1 megohm (plotter input).
A Moseley 7000A X-Y plotter was operated on X time base while the
spectrograph grating was driven at constant speed, thus giving the
spectral line structure as a function of wavelength. Noise problems


76
were minimized by the use of a low pass filter and by operating both
plotter and grating drive slowly enough to allow detailed plotting of
line shapes.
The system was grounded, using a 10-foot rod driven into earth
below the reactor. Braided copper strap was used for connections,
allowing no ground loops and using the stainless steel experimental
chamber as the main ground bus.
The following chapters will detail the use of the equipment
herein described and present results and analysis of the effects seen.


CHAPTER 4
ANALYSIS OF "iN-REACTOR" PLASMAS: FISSION
FRAGMENT GENERATED AND GLOW DISCHARGE
When referring to the photon output from the "in-reactor"
plasma, it can be assumed that the plasma is optically thin or that
there is very little absorption of photon energy by the gas. In order
to analyze the optical emissions and determine some characteristics of
the excited gas, some model is useful. Since it is presupposed that
the excited gas is in thermal nonequilibrium, the most valid model, as
previously stated, is a coupled set of interaction rate equations.
Without a complete set of cross section data for generation and decay
of excited states, this type of model is not useful. These data are
not available in complete form; therefore, the rate equation and com
bination type approaches [15] are by-passed in favor of a more easily
applied method, Boltzmann analysis.
The assumption that fission fragment excitation produces a gas
that is in thermal equilibrium, where the electron temperature and
distribution of excited states is defined by Fermi-Dirac or Boltzmann
statistics, is probably not valid. But, there are certain features of
this type of model that can prove useful in determining trends in the
excited state densities and in the search for a so-called "negative
temperature" or population inversion for pumping of a laser. The most
77


78
important feature of this model is the capability of describing the
plasma by an exponentially dependent factor analogous to the Boltzmann
temperature. Pressure-dependent plots of this factor and the excited
state densities from which it is derived are described in this chapter.
Also included is a review of all experimental fission fragment inter
action data generated by this research and an analysis of these data to
determine the characteristics of the generated plasmas. A review of
3 4
the experimental results of the He and He glow discharge reactor irra
diations is also included.
4.1 Experimental Procedure and Data Analysis:
Fission Fragment Interactions
The three gases bombarded with fission fragmentshelium, argon
and carbon tetrafluoridegave a luminous output that was easily mea
surable both for atomic spectral line peaks and for molecular band peaks.
Data were recorded by the methods described in Chapter 3. A typical
spectral sweep is shown in Figures 4-1 to 4-5 for helium at 100 torr
pressure. A second sweep is required with a different recorder sensi
tivity when the line or band intensity exceeds the plotter peak value
(Figure 4-1).
An interesting feature of these data is the significant back
ground produced by gamma interaction with the photomultiplier. This
background supplies the error in the spectral line intensity measurements.
The large amount of gamma shielding shown in the previous chapter reduced
this background to a tolerable level so that the measurement error on
the low level lines was acceptable. Other sources of error, such as
deviations in reactor operating power and changes in the nature of


79
j4so/- **> n.* /U** 3S~£ jm foo^s /40OCf*~*
3850 A -> 4410 A
.. *
A'f J hi
H-l*
2700 A + 3336 A
Figure 4-1 Helium Spectrum


80
0i4rtk lit1*7* //,*/**£*
410^*14 ,mt
** ££ ^
ro fc**t
ajj
3336 A + 3967 A
V/5"
i*
V. *
,|.\t<: H.71
3967 A -> 46 S
yif
Figure 4-2 Helium Spectrum


i***' no*/*'
81
Hi IS 4^ 5iV7
He'1 /*>1~
"if
* S
sv '
*>d
5247 A - 5877 A
Figure 4-3 Helium Spectrum


82
5877 A 6506 A
i
,-ar*
1'J' I "
f1 /.*
^V'
>'N
6506 A -> 7136 A
Figure 4-4 Helium Spectrum
U~ Li.


>4.
83
7136 A
7762 A
Figure 4-5 Helium Spectrum


84
the gas fill, were deemed insignificant in most cases and are noted
where applicable. Errors associated with the band height measurement
of CF^ and its reaction products cannot be established since the molec
ular dissociation and recombination of the various species present are
continuing kinetic processes reaching equilibrium in a long time
frame (about 3 hours).
At 100 KW reactor power, the error in the intensity is a con
stant factor equal to 1.125 mV divided by the appropriate calibration
factor for the wavelength of interest. This error (AI) is shown on the
linear intensity versus pressure plots. For the logarithmic calculation
of relative excited state densities, the error can be expressed as AF,
the standard error, where
and
Therefore,
and
AF
3f
ai
AI
(46)
(47)
(48)
(49)
This is the error indicated by the error bars on the
Boltzmann plots.
Calibration of the system was accomplished by using a tungsten
lamp calibrated by the National Bureau of Standards and a mockup of
the experimental system. All of the optical elements included in the


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UNIVERSITY OF FLORIDA
3 1262 07332 045 8
3 1262 07332 045 8


EXCITATION AND IONIZATION OF GASES
BY FISSION FRAGMENTS
By
ROY ALAN WALTERS
4 DISSERTATION PRESENTED TO THE GRADUATE COUNCIL OF
THE UNIVERSITY OF FLORIDA IN PARTIAL
FULFILLMENT 01 THE REQUIREMENTS FOR THE DEGREE OF
DOCTOR OF PHiLOSOPI./
UNIVERSITY OF FLORIDA
1973

bL-IZ-Z
To my father,
Harry Walters,
who was, in my eyes, the greatest of
engineers and the greatest of men.

ACKNOWLEDGMENTS
The author would like to express his deepest appreciation and
gratitude to Dr. Richard T. Schneider, the chairman of his supervisory
committee, for his guidance and support in this research, and for the
faith and friendship he showed toward the author throughout this
academic endeavor. Sincere thanks are extended to the other members
of the supervisory committee, Drs. Hugh D. Campbell, Kwan Chen, George
R. Dalton, and William H. Ellis.
The author also wishes to thank Dr. Edward Carroll for his
ideas and encouragement on the LMFBR detector studies.
Special note should be made of the valuable contributions of
Mr. Ernest Whitman, who aided the author with the design and construc¬
tion of the vacuum chamber, and of Mr. Richard Paternoster, who
developed the computer analysis and plotting programs. Thanks are
also extended to Mr. George Wheeler for his valuable assistance in the
construction of equipment and its operation.
The author acknowledges the technical assistance provided by
Mr. Henry Gogun and the other members of the UFTR crew.
Special thanks are extended to the author's wife and son for
their help in the production of this paper and for their patience and
support through the years this endeavor has taken to complete.
The author will be forever indebted to his father, the late
Harry Walters, for his unfailing faith and encouragement, and most
iii

especially, for his aid in the actual production of this manuscript.
Many of the diagrams that are a part of this dissertation are products
of his highly skilled hands.
Appreciation is expressed to Mrs. Edna Larrick for typing the
final draft of this manuscript.
This research was supported by NSA Grant NGL-10-005-089.
IV

TABLE OF CONTENTS
Page
ACKNOWLEDGMENTS iii
LIST OF TABLES viii
LIST OF FIGURES ix
ABSTRACT xiii
CHAPTER
1 INTRODUCTION 1
1.1 The Nuclear-Pumped Laser 1
1.2 Previous Studies of Fission
Fragment-Produced Plasmas . . 9
1.3 Glow Discharge Irradiation and Fission Fragment
Interaction Experiments 11
2 THEORETICAL CONSIDERATIONS 14
2.1 Energy Deposition by Fission Fragments
and Other Particles 14
2.2 Energy Deposition by the Reaction He^(n,p)T
in a Glow Discharge 37
2.3 Description of a Fission Fragment-Produced Plasma . 40
3 PLASMA RESEARCH APPARATUS 49
3.1 Introduction 49
3.2 Primary System 50
3.2.1 Plasma Region 51
3.2.2 Vacuum Chamber; Optical, Gas
and Electrical Feeds 55
3.3 Uranium Coatings 57
3.3.1 Coating Requirements 57
3.3.2 Coating Thickness 57
3.3.3 Review of Methods and Chemistry 60
3.3.4 Chemical Procedures 61
3.3.5 Mechanical Coating Procedure 63
v

TABLE OF CONTENTS (Continued)
CHAPTER Page
3 (Continued)
3.4 Support Systems 65
3.4.1 Reactor: Neutron Flux and Gamma Dose 65
3.4.2 Electrical Systems 67
3.4.3 Gas Filling Systems 68
3.4.4 Shielding 70
3.4.5 Safety 71
3.5 Data Acquisition Systems 75
4 ANALYSIS OF "iN-REACTOR" PLASMAS: FISSION FRAGMENT
GENERATED AND GLOW DISCHARGE 77
4.1 Experimental Procedure and Data Analysis:
Fission Fragment Interactions 78
4.2 Helium 86
4.2.1 Helium Kinetics and Spectral Analysis 88
4.2.2 Line Intensity and Excited State Density ... 92
4.2.3 Boltzmann Plot Analysis 102
4.2.4 Field Amplification of Line Intensities .... 110
4.3 £rgon Excitation by Fission Fragments 121
4.3.1 Argon Kinetics and Spectral Analysis 122
4.3.2 Line Intensity and Excited State Density . . . 131
4.3.3 Boltzmann Plot Analysis 135
4.3.4 Field Amplification 140
4.4 CF^ - Fission Fragment Interactions 153
4.5 Glow Discharge Irradiations 160
4.5.1 Experimental Procedures 161
4.5.2 The Glow Discharge 161
4.5.3 General Reactor Mixed Radiation Effects
on the Glow Discharge 164
4.5.4 Volume Deposition 171
4.5.5 Cathode Deposition 174
5 APPLICATIONS OF FISSION FRAGMENT-PRODUCED PLASMAS .... 178
5.1 The Nuclear-Pumped Laser 179
5.2 A Neutron Detector for the Liquid Metal
Fast Breeder Reactor 187
5.2.1 Diagnostic and Power Supply Systems 190
5.2.2 Neutron Detector Experimental Results 192
5.2.3 Data Projections and Realistic Chamber Design . 198
vi

TABLE OF CONTENTS (Continued)
CHAPTER Page
6 CONCLUSIONS 201
APPENDIX
I PRESSURE DEPENDENCE OF RELATIVE LINE INTENSITIES
AND EXCITED STATE DENSITIES - HELIUM 205
II BOLTZMANN TEMPERATURE PLOTS - HELIUM 223
III PRESSURE DEPENDENCE OF RELATIVE LINE INTENSITIES
AND EXCITED STATE DENSITIES - ARGON 231
IV BOLTZMANN TEMPERATURE PLOTS - ARGON 277
V FIELD AMPLIFICATION OF ARGON SPECTRAL EMISSION 295
BIBLIOGRAPHY 302
BIOGRAPHICAL SKETCH 308
vii

LIST OF TABLES
Table Page
4-1 HELIUM DATA 116
4-2 IDENTIFIED CASCADES OF ARGON II 134
4-3 ARGON DATA 145
4-4 CF FISSION FRAGMENT IRRADIATIONS:
BAND PEAKS OBSERVED AT 760 TORR 160
viii

LIST OF FIGURES
Figure Page
2-1 Geometry 21
2-2 Range of Fission Fragments in Helium and Argon 29
2-3 Deposition of Energy into Helium by Fission Fragments,
§ = 3.8 x 1011 —^ 33
cm -sec
2-4 Deposition of Energy into Argon by Fission Fragments,
$ = 3.8 x 1011 —~ 34
cm -sec
2-5 Energy Deposition by Fission Fragments in Argon
and Helium - A Fixed Cavity 36
3-1 Reactor Mounting 52
3-2 Chamber Experimental Sections 53
3-3 Chamber Detail - Reactor Region 54
3-4 University of Florida Training Reactor 56
3-5 K as a Function of Density 58
3-6 The Kinetic Energy of Fission Fragments as
a Function of Mass Number [38] 59
3-7 Chemical Procedures Coating Solution 62
3-8 Mechanical Procedures for Coating 64
3-9 Distribution of Thermal Neutron Flux
along Experimental Chamber 66
3-10 General Gas Discharge I-V Characteristic 69
3-11 Chamber Mounting and Shielding Cave 72
4-1 Helium Spectrum 79
'4-2 Helium Spectrum 80
xx

LIST OF FIGURES (Continued)
Figure Page
4-3 Helium Spectrum 81
4-4 Helium Spectrum 82
4-5 Helium Spectrum 83
4-6 Helium Excited States and Transitions 87
4-7 Optically Viewed Energy Deposition in Helium
and Argon as a Function of Pressure 95
4-8 Helium Intensity and Energy Deposition as
a Function of Pressure 97
4-9 Relative Excited State Population Density as
a Function of Pressure 98
4-10 Line Intensity versus Pressure - Helium 99
4-11 Boltzmann Plot - Helium Glow Discharge 104
4-12 Boltzmann Plot - Fission Fragment Excited Helium .... 105
4-13 Pressure Dependence of the Boltzmann Plot
Correlation Coefficients - Helium 107
4-14 Boltzmann Temperature as a Function of Pressure 108
4-15 Current-Voltage Characteristics of
Fission Fragment Excited Helium 112
4-16 Line Amplification and Current as a Function of
Applied Voltage - 30.5 cm Long Helium Cavity 114
4-17 Electron Energy Distribution - Fission Fragment
Excited Helium 120
4-18 Argon Spectrum 124
4-19 Argon Spectrum 125
4-20 Argon Spectrum 126
4-21 Argon Spectrum 127
4-22 Argon Spectrum 128
4-23 Argon Spectrum . 129
x

LIST OF FIGURES (Continued)
Figure Page
4-24 Intensity and Calculated Deposition (Viewed)
as a Function of Pressure 133
4-25 Boltzmann Temperature Plot 600 torr Argon I 137
4-26 Boltzmann Plot Argon II, 600 torr 138
4-27 Argon Temperature and Correlation Coefficient
versus Pressure 139
4-28 Amplification and Current versus Applied Voltage -
150 torr Argon 141
E
4-29 Amplification Coefficient versus —, Argon 143
4-30 Electron Density and Temperature versus Pressure - Argon . 148
4-31 Ion Pair Generation Rate as a Function
of Pressure - Argon 149
4-32 Electron Energy Distribution - Argon 151
4-33 Electron Energy Distribution - Argon 152
4-34 Glow Discharge through 5.5 torr CF^ - 2000 A -• 5087 A . . . 155
4-35 Band Peak Intensity of 100 torr CF4 as a Function of Time . 156
4-36 Spectrum of Fission Fragment Excited CF^,
760 torr - 2000 A - 5087 A 158
4-37 Spectrum of Fission Fragment Excited CF^,
760 torr - 2646 A - 3280 A 159
3
4-38 Glow Discharge I-V Characteristics for He -CO -N ,
8:1:1, 10 torr 165
4-39 I-V Characteristics for Hollow Cathode Glow Discharges . . 167
4-40 I-V Characteristics, 3.3 torr Glow Discharge,
Flat Cathode 168
4-41 Voltage Decay, Glow Discharge, for Reactor Shutdown -
Constant 1, 20 ma 169
4-42 Voltage Decay, Glow Discharge, for Reactor Shutdown -
Hollow Cathode 170
xi

LIST OF FIGURES (Continued)
Figure
5-1 Nuclear Pumped Laser
5-2 Nuclear-Pumped Laser Output
5-3 Cavity Design
5-4 LMFBR Neutron Detector Signal Flow
5-5 Amplification of Argon Line Intensity versus
Reactor Power
O
5-6 Ar I 6965 A Filtered Output Neutron Detector
5-7 Total Spectrum Signal - Neutron Detector . .
Page
181
184
186
191
194
195
196
5-8
P-P Voltage versus Reactor Power - Neutron Detector
197

Abstract of Dissertation Presented to the
Graduate Council of the University of Florida in Partial
Fulfillment of the Requirements for the Degree of Doctor of Philosophy
EXCITATION AND IONIZATION OF GASES
BY FISSION FRAGMENTS
By
Roy Alan Walters
June, 1973
Chairman: Dr. Richard T. Schneider
Major Department: Nuclear Engineering Sciences
The excitation and ionization produced by fission fragments was
investigated to identify basic mechanisms that could be applied to
direct nuclear pumping or enhancement of gas lasers.
A cylindrical U foil and its axial electrodes were placed
^oo
in a vacuum chamber which was capable of transmission of fluorescence to
o o
its exterior from 2000 A to 8000 A. The chamber was filled with argon,
helium or carbon tetrafluoride at various pressures and emersed in
11 2
a thermal neutron flux of 3.8 y 10 n/cm -sec.
The spectrum obtained from this excitation was qualitatively
similar to a glow discharge for argon and helium except for the pres¬
ence of excited ion species of He II and Ar III. The spectral output
from irradiation of 760 torr carbon tetra fluoride provided a band
system that is presently unidentified. Pressure dependent relative
intensity and excited state density data provide information on state
and species kinetics such as formation of molecular ions and their loss
Four possible population inversions were identified in
xi ii
mechanisms.

Ar II. Boltzmann analysis of the excited states supplied a temperature
for each species where the correlation coefficients of the fit lines
indicate that the plasmas are typical nonequilibrium cascade systems.
10-3
Electron densities around 10 e /cm and Maxwellian temperature
values for the collected electrons have been obtained from the recombina¬
tion region I-V characteristics. Electron energy distributions formu¬
lated from the data compare favorably with referenced calculations.
Ion pair generation rates were well within expected deviation compared
to calculations using a two-region energy deposition model.
In the ion chamber region of the I-V characteristics, line
emission increased as an exponential function of field strength.
A model for this amplification was developed for argon, utilizing an
amplification coefficient applicable to all pressures.
A neutron detector was developed for the liquid metal fast
breeder reactor by using optical transmission from the reactor core of
electric field modulated emission from fission fragment excitation.
Measurement of the modulated field effect eliminates the majority of
noise sources and gamma degradation signal loss associated with other
detectors.
Because of the excellent spectral output from Ar II, a nuclear
pumped argon ion optical cavity was constructed. Data from reactor
irradiation of the cavity indicate that it was lasing.
The effect of mixed radiation from the reactor on a glow dis-
11
charge was studied. For thermal neutron fluxes less than 3.8 X 10
2 7 3
n/cm -sec and gamma dose rates of 1.1 x 10 R/hr, irradiations of He ,
4
He , N and mixtures thereof show that there is no volume deposition
xiv

effect on the glow discharge. A cathode photoemission effect was found
that altered the balance of the discharge. Positive ion bombardment
3
from the He (n,p)T reaction products produced a considerable electron
source that perturbed the cathode fall region. Enhancement of CC>2 lasers
was showai to be a mechanism of preionization for low voltage glow dis¬
charge initiation and subsequent maintenance with lower power input.
This lowers the temperature of the discharge and improves laser pumping
efficiency.
xv

CHAPTER 1
INTRODUCTION
During the last decade, fission fragments and other energetic
heavy ions that are produced by neutron reactions have been examined
as possible sources of energy for generation of high temperature plas¬
mas. These high energy particles can be produced in great numbers in
a nuclear reactor where the reaction source (neutron flux) can range
17 2
up to 10 n/cm -sec in short pulses. The main thrust of research in
this area has been toward the demonstration of a nuclear-pumped laser.
1.1 The Nuclear-Pumped Laser
The term "Nuclear-Pumped Laser" refers to a laser that is
excited by products of nuclear reactions only and not by any electri¬
cal or optical source.
The link between the reactor and laser is natural when one
considers that communications could be greatly aided with transmission
of data to earth by laser beam in advanced extraterrestial equipment
which will have to include a nuclear reactor for power generation.
Direct coupling of a laser to a nuclear reactor is necessary
in order to produce desired high input powers. One might envision
a reactor-laser system where an optical cavity and the reactor fuel
235
are combined. A set of U internally coated tubes could be grouped
together in a cylindrical shape where the optical cavity would be
1

2
formed by mirrors reflecting through the tubes. A neutron moderator
would surround the tubes and cooling could be accomplished by passing
the laser gas through the tubes and then through a heat exchanger.
235
The fissioning of the U would supply both neutrons for sustaining
the nuclear reaction and fission fragments for excitation of the gas.
Each fission event supplies two fission fragments, a heavy fragment
with an average energy of 67.5 MeV and a light fragment with an aver¬
age energy of 98.7 MeV. These light and heavy fragments vary in weight
according to the familiar fission product distribution, but both frag¬
ments have the very important characteristic of being emitted with
a charge of about 20 e. This results in a very large coulombic inter¬
action rate and, thus, a very large deposition of energy in a small
path length, producing the excited states utilized in the laser.
Operating this reactor in a pulse mode will maximize the peak laser
power output.
Another nuclear-pumped laser scheme involves a gas core reactor
using UF as a fuel and some fluoride molecular species derived from
6
UF dissociation reactions as the lasing species. A similar homogen-
6
235
eous concept involves insertion of U compounds into a liquid dye
laser in order to produce a critical mass and thus a reactor. This
system would derive its excitation from fission fragments rather than
from chemical or optical sources. One disadvantage of the liquid dye
laser concept is the apparent breakdown of long chain dye molecules by
radiation interaction. R. Schneider [ 1 ] has inserted Rotemin b dis¬
solved in ethyl alcohol into a reactor and observed fluorescence.

3
When the dye was removed from the reactor, it was evident that it had
been completely destroyed, since there was no color, or fluorescence,
left in the liquid. Much experimental work has been done trying to
show the feasibility of a nuclear-pumped laser. To date, no proof has
been presented that confirms the operation of such a laser.
There are several alternatives when considering an energy
source for direct excitation of a laser. The most widely available
source is gamma radiation, but in order to effect efficient energy
transfer, high density solids must be used. A desire to optimize the
absorption led early workers [2,3] to concentrate on direct excitation
of solid state lasers. However, gamma radiation was found to suppress,
rather than aid, lasing action in all solids studied to date. This
"cutoff" phenomenon is generally attributed to radiation damage in the
solid.
An obvious solution to the problem of radiation damage is to
use a gas or liquid lasing medium. For gases, this implies the use of
a high energy heavy particle that has a large dE/'dx. Such a particle
is exemplified by the fission fragment. Liquid lasers are still in
their infancy and only one published report is available on an attempt
at nuclear pumping [4]. Nuclear pumping of gas lasers has been studied
extensively starting with a comprehensive study by L. Herwig [5] xn
1964. He recognized the radiation damage problem associated with
solids and decided to concentrate on gas laser nuclear pumping.
His calculations showed that He-Ne laser threshold requirements were
theoretically within the reach of some reactor and accelerator radiation

4
sources. Herwig also noted that a large diameter laser may be possible
due to the inherently low electron temperature expected in the radia¬
tion produced plasma.
J. DeShong [6] carried out more detailed calculations and
showed that a high pressure, large diameter nuclear-pumped laser has
theoretical efficiency two orders of magnitude greater than small diam¬
eter devices. In 1967 he undertook a series of experiments to verify
the feasibility of direct pumping. None of his devices showed proof of
lasing. Eerkins [7,8] decided to study noble gases as a possible lasing
medium because their high density allows a large dE/dx by the fission
fragment and because their ionization energy is low (E^ = 15.68 eV for
argon). Because recombination and dissociative recombination is ex¬
tremely efficient in a cold plasma, it was felt that the argon ion tran¬
sitions would exhibit a population inversion greater than that seen in
conventional electrically pumped lasers. Eerkins's source of energy
17 2
was a TRIGA pulsed reactor with fluxes up to 10 n/cm -sec. The
235
reactor neutrons interacted with a U coating on the laser tube wall
and produced a fission fragment-generated plasma. Boron-coated walls
10 7
were also tried, using the reaction B (n.oOLi , producing a plasma
utilizing the reaction product energy of 2.3 MeV. Although Eerkins
did not find any proof of lasing, he did generate a light output that
was quite intense. Guyot [9], concentrating on Ar and C02 lasers, also
did not find lasing in his experiments.
Nuclear-pumped laser experiments previously mentioned concen¬
trated on pumping with a highly energetic particle that was a result

5
of a neutron reaction with B or a fission event. These experiments
also concentrated the reacting material on tube walls while inserting
gas as a target for the particles. V. Andriakhin [10] attempted lasing
in an entirely different manner. He utilized the large neutron cross
3 3
section (5000b) of the He reaction [He (n,p)T + 760 keV] to provide
3
a source for excitation in a cavity filled with a gas mixture of He
and mercury vapor. His device generated light output of 10 mW, but no
proof of lasing was seen.
Several researchers (T. Ganley [11], F. Allario [121, H. Rhoads
[13]) noted the inability of others to generate a nuclear-pumped laser
and decided to look at the effects of several nuclear sources on an
3
operating laser. All of these studies involved the use of He as a
4
replacement for He in a He-C02~N2 laser gas mixture while operating
the laser in a nuclear reactor. It was felt that the high efficiency
3
of the C02 laser would allow maximum conversion of the He (n,p)T reac¬
tion energy, 760 keV, into laser output.
All three authors noted an increase in the efficiency of the
laser being irradiated in the reactor and, therefore, an increase in
laser output. Rhoads recognized this increased laser efficiency as an
increase of the glow discharge efficiency. He described this effect
as primarily due to the bombardment of the cathode surface by gammas
and He (n,p)T reaction products and thus an alteration in the cathode
fall equilibrium. The output of a C02 laser depends, among other
things, on the electron temperature, Te, of the plasma. Bullis [14]
has shown that the electron temperature for optimum pumping of a CC>2

6
laser is far below that resulting from normal glow discharge pumping.
The addition of the radiation source term to the cathode fall equilib¬
rium allows the operation of a glow discharge at much lower currents
and field strengths, allowing lower Te and much more efficient pumping.
This irradiation effect also allows operation of glow discharges at
much higher pressures than previously attainable.
It would also be possible to increase the power output of
present operating laser systems by the addition of a radiation source
at the cathode.
The glow discharge irradiation work described in this disserta¬
tion was done simultaneously with the nuclear-enhanced laser work de¬
scribed above; the results shown in this paper basically agree with
those described above.
Upon termination of the nuclear-pumped laser experiments, it
became evident that the theoretical considerations used to calculate
the neutron flux needed for lasing action may be inaccurate. The
thermal flux level available in many reactors is well above the calcu¬
lated lasing thresholds; therefore, some of the experimental devices
should have lased. Most of the theoretical work has been based on the
premise that one excited state is available for each 100 eV deposited
in the gas [5,6], This relation results from the assumption that once
the energy is deposited in a gas by nuclear interactions, subsequent
distribution of excited states, ionization, etc., is identical to that
of electrically pumped lasers.

7
G. R. Russell [15,16] has noted - at least for the case of
atomic argon - direct nuclear excitation of gases is an entirely dif¬
ferent kinetic process than that found in most CW electrically excited
lasers. Generally, in electrically pumped gas lasers population inver¬
sions are formed by metastable state collisions with ground state atoms
(He-Ne) or other energy transfer systems initiated by the electron
swarm.
The kinetics of the argon ion laser, where the population
inversion is produced by electron collisional excitation of the upper
state and electron recombination in the lower state, served as Russell's
example. On the average, it takes two collisions with electrons to
elevate the argon ground state to the ionized excited level required
for population inversion. Such a ladder-climbing system is not evident
in the low temperature plasma generated by nuclear sources. This low
temperature system is more analogous to a recombining plasma at low
thermal electron temperatures, where there is additional preferential
excitation due to high energy particles superimposed on the thermal
excitation. Therefore, it would not be expected that inversions formed
in electrically excited CW lasers would necessarily be found in nuclear-
excited lasers. It is also very probable that the additional excita¬
tion due to high energy heavy particles will create new inversions not
previously observed in electrically excited lasers.
Russell supports this last premise by calculating population
inversions produced in argon by fission fragment interactions and not
available in conventionally pumped lasers. His calculations included

8
formation of excited states due to recombination of thermal electrons
and the associated radiative and collisional decay of these states.
To complicate matters further, Miley [17] and others have indicated
that there is a difference between how fission fragments and alpha
particles lose their energy in a gas medium. This is because alpha
particles remain essentially charge invariant over their path length,
while fission fragments - starting with an average charge of 20e - lose
their charge by recombination while losing energy by coulombic, rather
than nuclear, elastic collisions. Recently several of the authors [ 1]
mentioned above have revealed that they now feel that once the fission
fragment deposits its energy into a gas, this excited gas may be
regarded as identical to the electrically excited gas.
From the above discussion it can be concluded that the exact
nature of a gas excited by fission fragments is not known. Also, there
is a distinct possibility of producing a nuclear-pumped laser using
some unusual (not normally available) population inversion; some gas
now known to exhibit population inversions may become the standard for
this type of laser. A less optimistic conclusion is that nuclear
pumping is not presently feasible.
No one has previously studied experimentally the excited
states of a plasma produced by an extremely large source of heavy,
highly charged particles such as fission fragments. Until detailed
analysis of heavy particle-produced plasmas is complete, the nuclear-
pumped laser experiments are without foundation.

9
1.2 Previous Studies of Fission
Fragment-Produced Plasmas
To study excited states of atomic and ionized species exper¬
imentally, spectrographic analysis of the spontaneous photon emission
from these states is necessary.
Several researchers have studied experimentally alpha particle-
induced luminescence of gases with great success. S. Dondes et al. [18]
have been able to supply very good spectrographic plates (long time
210
exposures) of many gases exposed to a Po ,5 MeV, alpha source.
Amplification of the gross light output was indicated upon placing a
350 V/'cm field across the luminescing area. P. Thiess [19] , using
a similar - but more powerful - source and photon counting techniques,
was able to obtain similar data. Other allied work has come from the
French gas counter research program [2o,21,22,23] and two very early
studies [24,2 5], These latter experimental works used sources of very
low intensity and the data were decidedly biased toward use in the
design of counting equipment. The source strengths used in all of
the alpha particle interaction work are weak enough, and the electron
density therefore small enough, that the gas should probably be described
as a scintillating light source rather than a plasma. As mentioned
previously, it is hard to draw comparisons between such low level
a source luminescence and a plasma generated by a large fission frag¬
ment source, but these studies do give basic knowledge of the kinetics
of heavy particle interactions.
In contrast to excited state measurements, fairly extensive
measurements of electron densities in radiation-produced plasmas have

10
been reported. Jamerson et al. [26,27] worked with "in-reactor" fission
fragment-produced plasmas where, utilizing the I-V curves produced by
a field across the plasma, they were able to calculate values for
12 2
electron temperature and density. For a flux of 10 n/cm -sec a 600°K
electron temperature was found which compares favorably with the micro-
wave cavity measurements of Bhattacharya [28]. Ellis et al. [29,30,31],
3
have studied recombination coefficients in plasmas produced by He reac¬
tion products, alpha particles, and fission fragments, and have added
immensely to the knowledge of the kinetics of these plasmas.
The above works indicate that the general kinetics studies of
alpha and fission fragment-produced plasmas are no longer in their
infancy; therefore, one can draw' on these data in explaining the source
terms for generating atomic excited states.
A very large library of cross sections for collision-produced
excited states is available in a book by E. W. Thomas [32]. These
cross sections have been generated by bombarding various gases by heavy
ions produced in accelerators. Unfortunately, none of the ions had
energies above 1.5 MeV and few had energies above 0.5 MeV. The appli¬
cability of these cross section data to fission fragment interactions is
questionable, but certain techniques used to generate these data are
of great interest in this study.
Several researchers have attempted to study spectral emissions
from fission fragment plasmas. F. Morse et al. [33] studied the
luminescence of several gases under bombardment by fission fragments
in a nuclear reactor. They did see some line structure, but concluded

11
that it was too weak to study (96-hour exposures!). They then returned
to the use of alpha sources [18] where reactor associated problems were
not present. R. Axtmann [34] studied the luminescent intensity of
252
nitrogen bombarded by fission fragments from Cf , but he just assumed
that the light was from the second positive system of molecular nitro¬
gen emission and tried no spectroscopic analysis. The above studies
led Pagano [35] to attempt spectroscopic analysis of various gases
252
bombarded by Cf fission fragments, but his source was not strong
enough to allow recording of spectra.
During the nuclear-pumped laser studies of Eerkins [7,8],
several spectroscopic plates of their pulsed plasma were taken, but
at that time they were more interested in producing a laser than study¬
ing the plasma that they assumed contained population inversions.
Thus, the spectroscopic work was limited to a few plates in which the
photon output was filtered by the mirrors of the laser system.
The above spectroscopic studies gave great encouragement to
this author in his studies of "in-core" fission fragment-produced
plasmas. After careful analysis of the techniques used by these
researchers, a set of experimental guidelines (see Chapter 3) were
generated in order to avoid the known problems associated with such
research.
1.3 Glow Discharge Irradiation and
Fission Fragment Interaction Experiments
The need for experimental data on fission fragment-produced
plasmas and on the radiation-produced changes in an already existing
plasma has been established. The dual purpose of this dissertation

12
is to fill some of this unknown area and to generate sound techniques
for the study of "in-reactor" particle produced plasmas. Fortunately,
as will be shown in the following chapters, one basic experimental
apparatus can be used for this dual purpose.
The first probe into this area involves the study of a known
plasma, the glow discharge, and what happens to its operation under
3
bombardment by gamma and reaction products of the He (n,p)T reaction.
Several cathode configurations and several gases are studied for their
response to the reactor sources. Conclusions are drawn as to the extent
of changes and how they occur.
The most difficult area, the investigation of fission fragment-
produced excitation, is presented utilizing the assumption that the
plasma is an interacting Maxwellian system. The analysis of the data
emphasizes the deviations from equilibrium of this system. This approach
was taken due to the availability of large numbers (45 Ar II spectral
lines) of easily measurable spectral lines emitted by atomic as well as
4
ion species of several gases. He , Ar, and CF^ were studied for pos¬
sible population inversions by using Boltzmann plot techniques and
analysis of deviations of excited state populations as a function of
pressure. Data are supplied on the effect of pressure and a DC field
on the intensity of line emission.
A unique neutron detector for the liquid metal fast breeder
reactor was suggested by Dr. Edward E. Carroll [36]. Drawing from the
above data, a detection system was developed and tested using electric
field amplified light variations as a basis for its operation. Also,
an argon ion laser was tested utilizing pumping by fission fragment

13
interactions only. Results from this device, although not proof of las¬
ing, show promise for future investigators.
In summary, this chapter has outlined the great need for
experimental data on the nature of effects of mixed radiation sources
on a glow discharge and has shown why the study of fission fragment-
produced plasmas is necessary.

CHAPTER 2
THEORETICAL CONSIDERATIONS
To assess adequately the effects observed in the experimental
procedure, certain theoretical considerations must be made. The two
basic considerations that will be reviewed in this chapter are, first,
the way a particle deposits its energy, and, second, how this energy
might be distributed in a plasma. Basic calculational techniques will
also be reviewed for use in analysis of the data described later in
this study.
2.1 Energy Deposition by Fission Fragments
and Other Particles
The passage of charged particles through matter has been
studied for at least half a century. It is not surprising that the
theoretical and experimental description of alpha-particle and proton
penetration phenomena is well advanced as these are the charged particles
with which most experiments were performed before the discovery of nu¬
clear fission. Presently there is emphasis on the study of the inter¬
action of ions with larger mass and charge than these elemental par¬
ticles. It is common practice to label ions such as fission fragments
as "heavy ions” in order to distinguish them from light ions such as
protons and alpha particles. This distinction is strictly arbitrary
since most of the phenomena involved in energy deposition by these
14

15
particles are identical. Fission fragments distinguish themselves as
heavy ions because they are very massive and have, immediately after
formation, about twenty electrons stripped from their atoms. Thus, the
effective charge of these fragments is considerably higher than those
of the light ion group. This is an important distinction, since heavy
ions suffer coulombic interactions, as well as the nuclear elastic
scattering found in light ion interactions. A light ion is essentially
charge invariant over its path length, while the fission fragment is
charge variable over part of its path.
The life of a fission fragment or other heavy particle is
summarized by Northcliffe [37]. If an atom is given a velocity greatly
in excess of the orbital velocities of its electrons and allowed to
enter a material medium, these electrons will be stripped from the atom
and the bare nucleus will proceed through the medium, gradually losing
energy because of coulornbic interactions with the electrons of the
medium. At this point, where the heavy particle velocity is high,
elastic or inelastic collisions with the nuclei of the medium will be
relatively rare and will add little to the energy loss process. At
first there is a small, but finite, probability that the ion will cap¬
ture an electron in one of these collisions and a large probability
that the electron will be lost in the next collision; but as the ion
slows down and approaches velocities comparable with the orbital veloc¬
ity of a captured electron, the capture probability increases and the
loss probability decreases. As the ion slows to velocities smaller
than the orbital velocity of the first captured electron, the capture
probability becomes very large and the loss probability approaches zero.

16
Meanwhile the probability of capturing a second electron grows and the
corresponding loss probability decreases, so that with increasing prob¬
ability the second electron is retained. As the velocity decrease con¬
tinues, a third electron is captured in the same gradual way, and then
a fourth, and so on. The major difference in the description of the
capture process for successive electrons is the change in velocity
scale necessary to match the progressive decrease of orbital velocity
of these electrons within the ion.
Eventually the ion reaches velocities smaller than the orbital
velocity of the least tightly bound electron and spends most of its
time as a neutral atom. By this time its kinetic energy is being
dissipated predominately by the energy transfer arising from elastic
collisions between the screened nuclear fields of the ion and atom,
and a diminishing amount of energy is being transferred to the atomic
electrons. The neutralized ion is said to be stopped when it either
reaches thermal velocities or combines chemically with the atoms of the
stopping material.
With respect to the medium into which the heavy particle or
fission fragment is penetrating, most of the ionization and excita¬
tion is caused by secondary electrons (delta rays) produced during the
initial coulombic stripping and recombination interactions. This does
not hold true, though, for a fission fragment near the end of its track,
where it is essentially neutral.
To calculate the space dependent deposition of energy in a
medium, it is usual to start with a stopping power relation. Using
appropriate geometry, one first calculates the available energy per

17
unit volume, and then using ion or excited state generating terms, the
kinetics of the system. The Bohr stopping equation for fission frag¬
ments is [3 8]
" S = 2TTNZeff ^2 Le + 2ttNZiZ2 ~2 Lv ’
mv
m2v
(1)
where
_ rot (3 -1/3 1 -1
L = L (— x + - x
e e \4 4
* (*A N = atom density of the density stopping material
M^,Z^ = mass and nuclear charge of the moving fragment
M_,Z = mass and nuclear charge of the stopping material
e,m = electronic charge and mass
v = velocity of the moving fragment
effective charge of the fission fragment example:
Z
eff
„l/3 .
. .. = Z v/v
eff o
.8
v =
x =
L =
L =
velocity of a Bohr-orbit electron (2.2 x 10 cm/sec)
’ v
2Z —
eff v
term for electronic stopping power
term for nuclear stopping power
L = the electronic stopping power for a particles of comparable
e
-8
velocities (about 6.33 x 10 v).

18
The first term in the right-hand side of equation (1) describes
the electronic stopping power derived from coulombic interactions.
The second term describes energy transfer by nuclear elastic inter¬
actions. It is standard practice to ignore the second term since the
amount of energy deposited by nuclear interactions is small compared
to the total energy deposited. Thus, using the first term only of
equation (1), the range of a fission fragment can be determined.
1 2
Assuming for the particle that E = — M v and that the Thomas-Fermi
1/3
effective charge, Z ^ = Z v/vq, is va]-icl> the fragment velocity
follows from equation (1) as
dv
dx
K(N,Z1,M1) ,
where
K(N,Z1,M1)
= 2trN
4 -8
e 6.33 x 10
,1/3
mv
8M-
6Z„
.2/9
.1/3
+ 1
(2)
(3)
K is therefore a function of the mass and charge of the moving
fragment and the density of the medium, but is velocity and space inde¬
pendent. Solving this equation shows that
v(x) = v. - Kx .
(4)
Solving this velocity-distance relationship for x when
v(x) = 0 or v(x)i = 0, where R equals the range of a particle
I x=R
with initial velocity v , the result is
R(v. )
i
v.
i
IT
(5)

19
Assuming the initial energy = — M v^ anc* substituting into
equation (4) produces the well-known square law energy deposition rela¬
tionship of a fission fragment,
E(x) = E.(l - |)
2
(6)
This relationship is therefore equivalent to the Bohr stopping
power equation using the Thomas-Fermi approximation for Z __ with the
efx
nuclear stopping term neglected.
Several authors' using the general equation,
E = E.(1 - £)“ , (7)
1 K
have disagreed with the n=2 value derived above. Axtmann [34], using
the luminescence of nitrogen under fission fragment bombardment, found
n equal to 1.7. Long [39] used n= 1 for his calculations where the
n value was obtained from collated range-energy data for a variety of
stopping materials. Steele [40] used n=1.5 to compute energy deposi¬
tion by fission fragments in water.
To generalize the square law equation (6) for a point source
in an infinite homogeneous medium, an energy transfer function can be
stated as
G(x, p) = E. (1 - —)
1 pR
(8)
where cos p is the angle between the x-axis and the direction of
particle movement.
To calculate the deposition in a gas by a fission fragment,
one must remember that a fission fragment source such as a coating of

20
U„0 has a finite thickness. The foil is a dense medium and thus
O O
absorbs a large amount of the fission energy available. Calculations
should therefore include this second medium unless the fuel is in a
gaseous form, such as UF^. It is very tempting to assume that only
perhaps one-half of the energy available v/ill get through the foil
into the gas. This assumption would be hard to prove because of the
difficulty of relating a measurement of this energy in one particular
experiment to a calculation where either the thickness or the density
of the uranium compound is different.
To calculate energy deposition at any point z of Figure 2.1,
one first assumes that scattering of the fission fragment by the medium
is negligible and that only straight line paths need be considered.
The origin of the geometry is at the left face of the source slab which
has a thickness R^, the range of a fission fragment in the source medium.
When x is larger than , the substitution z.- x - R^ is made so that
z = 0 at the interface. The source is assumed isotropic in emission
with azimuthal symmetry about x. The angle between the path and the
x-axis is 0 . The slowing down of the particle in both media is
described by equation (4). While the fragment is in medium I moving along
the abscissa, the residual velocity at x , v (x^x), of a particle borne
at x with initial velocity v^ is
v^x' ;x) = vi - kJx' - x| x < x' < R1 (9)
while for medium II
v2(z;x) = C(x) - K2z ,
(10)

Figure 2-1 Geometry

22
where C(x) is the residual velocity at z = 0 or the interface of a
particle born at x in medium I. Assuming continuity at the interface,
V* ;X>|x'=E1 = V2(Z;X)|Z=0
then
C(x)
Vi “ K1(R1 " X)
(ID
and thus, the residual velocity in medium II is
v2(z;x) = v± - K^R - x) - K£z
(12)
Since the thickness of medium I is equal to the range of a
fragment in medium I, equation (11) is valid for any 0 < x < R^.
For a fission fragment not moving along the abscissa, but in the
direction 8 = cos ^p,equation (12) becomes
(R1_X) z
v2(z;n,x) = v. - Kx —— - K2 - .
(13)
provided that
(Rrx) z
K, + K0 — < v for all p > 0
1 p 2 p - o
or, in other words, provided that the particle arrives in medium II.
Since it was previously shown in equation (5) that
one can state that

23
r r1-x z
v2(z;1i.,x) = V¿1 - — - -¡l-J .
(14)
The Energy Transfer Function of equation (8) can now be stated as the
two-medium function
1 2
F(z;|i,x) = - M1v2(z;|i,x)
r _ (Ri~x) _ z ~]2
Ei L
(15)
In order to eliminate the dependence on , a conversion factor a is
derived from the Bragg-Kleeman rule which converts the range of a
charged particle in one medium to its range in another medium.
Therefore,
and
where
and
r2 = r2 (VV1/2 Ri •
R2 = aRl
a = — (A /A )'1/2
P2 2 1
(16)
(17)
p = density,
A = atomic weight.
"a" may also be derived from the theoretical stopping equation
or from experimental measurements. Equation (14) thus becomes
r (R-.-x) ~i ~
G(z;|i,x) = E 1 %—\ . (18)

24
From the general geometry of Figure 2-1, a total energy current
is derived for a point r in medium II due to the source S(ro,Eo>Q) in
medium I.
Vr>=/ drQ f f dE0S(ro’Eo’™ G(r;ro’Eo’
1 o E
Q o
(19)
where
r = a spacial point in medium I,
o
"4
r = a spacial point in medium II,
Q = a solid angle characterizing the direc¬
tional distribution of the source,
E = initial energy of the fission fragment.
S(r ,E ,Q)dr dE dfi
o o o o
= the distribution of the fission fragment
source at r in dr , at fi in dfi and
o o
at E in dE (usually a constant).
o o
G(r;ro,EQ,Q) = the energy at r, carried by a fragment
—♦
originated at r , moving in direction 0
with initial energy E , assuming no
scattering.
If it is assumed that C(x) is the fission density,
C(x) = Zf(x)9(x), and that f(EQ) is the normalized fission fragment
spectrum, then with isotropic emission, the differential source within
a thin layer dx at x, emitted in the solid angle width dpdcp with
initial energy E in dE is
o o
C
S(x,E ,n,cp)dx dE dudcp = — f (E )dx dE d^dcp .
’ o o 4tt o o
(20)

25
Using the energy transfer function of equation (18) and equation (20)
in (19), one obtains the total energy current at z in medium II,
J (z), resulting from a distributed source of fission fragments in
E
medium I
Vz)
_1_
4tt
2rr
dE f(E )E
o o o
o
R1
*
dx
'¿/a
dp£(x)
aR^-ax+2
aR~
(Rj-x)
- —)
aR ) ’
(21)
Nguyen [38] discusses the limits of integration and how one
would analytically integrate this function. With a constant fission
density of C
CE R
P
VZ) = 2
1 Ti ^ 1 ,2 2 1.3 3 2 2 . .1
— ! — - bz + — b z +^bz -bz Q,n (bz) J
energy
2 1
cm -sec
(22)
where
b =
1 _ _1_
aRl R2
R and R being the ranges of fission fragments in mediums I and II,
1 Z
respectively, of a fragment having the initial energy E^. The required
boundary condition J,,(z)| =0 (or at bz = 1) is satisfied.
E Ur2
Equation (22) represents the total residual energy at point z.
The instantaneous energy loss per volume as a function of z is obtained
by taking the derivative of J^iz) with respect to z.
E

26
Vz)
CE R
P
dz
10
. 3 2
b z
- 2b2z
S/n (bz)
-]
energy
3
cm -sec
(23)
An almost identical empirical energy deposition relationship can be
derived, as previously noted, based upon the relationship
E(x) = E
i - 2
R
n
1 < n < 3 .
(24)
Both equations give similar results for small z, but vary considerably
for z approaching the range Rin medium II.
This energy deposition function ignores any nuclear elastic
collisions; but if one calculates an ion production source, a so-called
"ionization defect" takes into account this nuclear deposition, which
is less effective in ionization than coulombic interactions.
At this point researchers split to several different techniques
for generating source terms for a kinetic system. Most studies have
constructed an ion source term and used the standard w values for
fission fragment interaction with various gases. These values include
the "ionization defect" and are experimental in origin.
Using the square law point deposition form of equation (23),
one can derive, simply by dividing by w, the volumetric ion production
rate.
I.
i
1
dJ (z)
E
w. dz
i
CE .R
Pi
2w
i
Aiiv
H . L 1
2 2 2
z - 2b. z B/n b. z
i i
ion pairs
3
cm -sec
(25)
where the distinction is made between the light and heavy groups of
fission fragments. Therefore,
V2> = \ Vz) + I Vz> •
(26)

27
The assumption that w — is a constant value over the
ion pair
entire path of the fragment is false, but if one includes the "ioniza¬
tion defect” and views the target as a whole, such as a plasma system,
this approximation should be close to the actual generation rate.
P. Thiess [17] approached the problem in an unusual manner. Using
the semiempirical energy deposition approach, a suggested alternative
shown above, he avoids the use of w values by calculating excited states
and inoization directly. This approach requires knowledge of a complete
set of cross sections for generating the source terms for excited levels.
Thiess used modified Bethe-Born cross section data based upon proton
impact. Russell [16] used another approximation, the Gryzinski electron
interaction cross section, for his excited state calculations. Both
authors clearly state that the use of these cross sections may be
entirely invalid, but must be used because there are no experimentally
measured cross section data available for such interactions. One factor
that may make the Gryzinski electron interaction approximation more
applicable than the others is the fact that about two-thirds of the
ionization and excitation is distributed to the gas by secondary delta
rays or fast electrons, rather than by the primary fission fragment
particle.
The range of a fission fragment in a gas is a function of the
density of that gas and its molecular weight. Range relations are
strictly empirical and are derived from measured data independent of
straggling or other statistical phenomena.

28
Range as a function of pressure can be calculated using the
following equation [41]
R(cm)
where K = 1.4 for most gases (Figure 3-5).
Figure 2-2 shows a plot of range vs. pressure for both the
light group (E = 98.7 MeV) and heavy group (Eq = 67.5 MeV) fission
fragments in argon and helium.
Experimental procedures such as those used in this dissertation
are based on cylindrical geometry. The average chord length
(s ss 4 volume/area) best represents the distance that a particle—if born
on the surface or in the volume of the cylinder—would travel in a
straight line before it would collide with the surface. For a cylinder
30.5 cm in length and 3.7 cm in diameter, the average chord length
is 3.4 cm. These lengths are identical to those found in the experi¬
mental apparatus used here. It is interesting to note in Figure 2-2
that at all pressures below 1 atmosphere (760 torr), the range of
fission fragments in helium is greater than the average chord length.
The situation for argon is different since it is ten times as dense for
equal pressures; therefore, the average chord length is equal to the
range of the light fragment at 360 torr and equal to the range of the
heavy fragment at 280 torr. A quick conclusion could be that for most
of the experimental data that one would observe, only a small fraction
of the fission fragment energy would be deposited in the gas. This is
not necessarily true, because the energy deposition from the foil is

RANGE (cm)
29
Figure 2-2 Range of Fission Fragments
in Helium and Argon

30
skewed towards the foil surface due to the finite thickness of the
source and the fact that the great majority of the fission fragments
do not leave the source surface with the typical 67.5 MeV or 98.7 MeV
average energies that they are born with.
A much better view of the energy deposition can be gained by
calculating the deposition profile at each pressure. A calculation
of the energy deposition utilizes the square law deposition function
and geometry used for equation (23). First, several assumptions must
be made in order to equate the slab geometry calculation to the cylin¬
drical geometry that is presented in most experimental situations.
1. The slab and cylindrical two-region energy current functions
are essentially identical.
This is a good approximation since the range of a fission frag¬
ment in the U„0 source foil used in these calculations is only
O O
-4
7.5 x 10 cm; therefore, the great majority of the energetic fission
fragments that have a considerable range are emitted perpendicularly
from the surface.
2. Little energy is emitted to the gas when a fission fragment
collides with a surface.
This assumption is not adequate for exact analysis but should
be valid for the accuracy required here.
3. Energy deposition by other sources is a very small fraction
of the fission fragment deposition.
This assumption has been proved experimentally to be valid
by Leffert [26] , where he has shown that other sources, such as gamma

31
radiation, deposit less than 1 per cent of the total energy to a volume
in normal reactor situations.
In order to proceed further, the fission rate must be calcu¬
lated as follows:
C = Rf = N a § = E $
(27)
N = number density of target nuclei
CT = fission cross section
§ = average neutron flux along the foil
E = macroscopic cross section.
For these conditions,
2
Thickness =6.2 mg/cm (the range of a fission
fragment in U 0 )
O O
Average thermal flux = 3.8 x 10^ ——
cm -sec
Fission cross section = 505 barns 93% enriched uranium
the generating function per cm surface area is 8.06 x 10
11 fissions
2
cm -sec
From equation (23)
i=l,2
(28)

32
where
E
P
b
i
fission rate
most probable energy at birth
R
aR_
2i "li
fission fragment group.
(each group)
This generating formula is calculated by splitting the depend¬
ence on light and heavy particles, then adding the results, giving the
energy deposition profile shown in Figure 2-3 for helium and Figure 2-4
for argon.
The gas pressure, or atom number density, is the most important
factor in the deposition of energy in a fixed cavity. For pressures
below 760 torr in helium, the energy deposition across a 3.4 cm average
chord length cavity is approximately uniform. But, in argon, only
below 75 torr is the energy deposition somewhat uniform across the
cavity. Since this calculation takes into account only coulombic inter¬
actions and ignores the nuclear elastic and inelastic scattering of the
particles when they reach the neutral status, the energy deposition
curves fall off extremely fast. If the nuclear scattering terms were
included, the range would be extended slightly, but only a small addi¬
tion would be made to the deposition of energy at the end point of the
fission fragment path. The effect on the total deposition would also
be small [37],
One of the unknowns, as previously described, involves how the
energy is utilized, what excited states or ions are produced, and what

DEPOSITED ENERGY (MeV/cm -sec)
33
10° 101 102 103
DISTANCE FROM U308 FOIL, Z (cm)
Figure 2-3 Deposition of Energy into Helium
by Fission Fragments, $ = 3.8x10^ 2—
cm^-sec

DEPOSITED ENERGY (MeV/cm -sec)
34
DISTANCE FROM l^Og FOIL, Z (cm)
Figure 2-4
Deposition of Energy into Argon ^
by Fission Fragments, $ = 3.8x10 —
cmz-sec

35
photon emissions are coming from the "plasma." These items are
a function of cross section for the various species that are present
in the gas. Measurements of the photon emission of the gas are based
on total emission from the optical cavity; thus, this photon output
can be compared to the total energy deposited into the gas in this
cavity. A description of the total energy input can be obtained by
integrating the energy deposition function over all source areas and
over the average chord length. From equation (23),
E =
dA
dJE(z)
dz
dz
„ A CE R o o 9
E = j - lb z - 2b z Sm (bz)
-]
dz ,
where
z = average chord length, or
z = R2, if R2 < z
i = R = range of fission fragments in gas and is
b 2
a function of pressure.
Integrating,
z
MeV
sec
o
E =
/i n
f P
b z° 2 2
— b z (fa bz
Â¥
bz^J
(29)
(30)
(31)
Again, as in equation (28), the calculation is split for each
group of fission fragments. Figure 2-5 shows the solution of equa¬
tion (31), where E is calculated as a function of the gas pressure for

ENERGY DEPOSITION (MeV/sec)
36
101 102 103
PRESSURE (torr)
Figure 2-5 Energy Deposition by Fission
Fragments in Argon and Helium
- A Fixed Cavity -

37
the representative cylinder with an average chord length of 3.4 cm.
The deposition in the cavity filled with helium is almost a linear
function of pressure. In argon, the effect of the range being less
than the cavity dimensions is evident by the leveling off of the curve
above 200 torr. Depending on the recombination and diffusion of elec¬
trons at pressures above 200 torr, the fission fragment-produced
excitation may generate a torroidal luminescent output in the cylin¬
drical cavity. This would alter the uniformity of the photon output
into the fixed solid angle view of the diagnostic equipment and may
provide erroneous data, especially if some of the surface region were
optically shielded from the detector system. It is estimated that such
a shading effect exists in the experimental equipment associated with
this work. Further review of this problem can be found in Chapter 4.
3
2.2 Energy Deposition by the Reaction He (n,p)T
in a Glow Discharge
3
High energy products of the reaction He (n,p)T are of interest
3
here because of the use of He in the glow discharge experiments to be
described later.
The proton and triton share the reaction energy of 760 keV with
the heavier triton taking 190 keV and the proton 570 keV. The initiat¬
ing neutron energy is in the range of less than a few eV; therefore,
little momentum is transferred and the reaction particles travel
randomly in opposite directions. Thus, the interactions with the gas
are independent of one another.

38
Fortunately, the linear stopping power formulation for protons
and heavy-heavy protons (tritons) has been established as satisfactory
for calculating energy loss phenomena. Interesting calculations for
this reaction include total energy deposited in the cylindrical glow
discharge and total ionization produced by this deposition. These
3
calculations are done assuming that the gas is He at a pressure of
dE
15 torr for an 8:1:1 mixture of He-CO -N„ is 2.6 times that of
dx 2 2
helium [13]; therefore, the calculation of total energy deposited
should be multiplied by this amount for experiments involving C02 gas
mixtures. Reference 8 gives the stopping power of helium as
dE
—^ = 105
dx
eV
for
570
keV
protons,
cm-torr
dE_
T
970
eV
for
190
keV
tritons.
dx
cm-torr
For a cylindrical cavity 3.7 cm in diameter and 12.7 cm long
(identical to the dimensions of the experimental apparatus) the average
chord length is 2.87 cm.
The total energy deposition is calculated using the following
equations:
1. Reaction rate
_3
R = N^ct$ cm (32)
3
where N = number density of He atoms
c = thermal neutron cross section = 5400 b
11 2
$ = thermal neutron flux - 3.8 X 10 n/cm -sec.

39
where
P
V
Total energy deposition
-[(f)
p T
= average chord = 2.87 cm
= pressure = 15 torr
3
= volume = 136 cm .
eV
sec
(33)
3. Total energy available
keV
E = (760 keV) RV
sec
(34)
Upon application of the data to these equations, it is found
13 eV
that only 1.75 x 10 —— is being deposited into the cavity. This is
14 eV
only one-tenth of the total available energy, 1.12 x 10 , generated
-6
in the cylindrical volume.
This energy input is equal to only 2.8 x 10 _ watts, so the
total energy both available and deposited at this neutron flux level
is but a small fraction of the energy deposited by electrical excitation.
In fact, measurements that will be detailed in Chapter 4 for glow dis¬
charges show that the minimum electrical power input needed to generate
a glow discharge in such a cavity is 0.5 watt. The one conclusion that
can be drawn from the calculations is that volume ionization or excita-
3
tion by He reaction products probably does not account for any signif¬
icant changes in the operation of typical low power glow discharges,
12 2
especially for neutron fluxes below 10 n/cm -sec.
Butler and Buckingham [42] state that for high energy ions
whose velocity is much greater than the thermal ion or electron

40
velocity, the loss rate of energy to the electrons is larger than to
2 3
ions by the factor (m./m )(p /z. p.). For He this ratio is approx-
i 0 e i i
imately 20. This could account for some volume enhancement of energy,
especially in the case of fission fragment deposition. But, and
p. are extremely small in both cases and most of the energy transfer
is to neutral particles. This effect then, is not significant in the
tenuous plasmas described here. Since it has been established [11,13]
that the nuclear reactor does affect the operation of a glow discharge
and thus laser operation, the changes occurring must be a function of
either changes in glow discharge structure or irradiation of the elec¬
trodes. Data describing these effects are presented in Chapter 4.
2.3 Description of a Fission Fragment-
Produced Plasma
At present much effort is being expended in the area of char¬
acterization of the tenuous "plasma" produced by fission fragment
sources [ 1 ]. The assembly of a set of kinetic rate equations is the
ideal approach to the characterization of this gas. But, because of
this method's detailed description of the number density of all species
and their important excited states, all reaction cross sections must
be known. Considering the number of species of a gas (atoms, ions, and
molecular combinations) and the excited states possibly present in
these species, this becomes an arduous task.
In most experimental processes, a small amount of impurity
gases are always present. These impurities enter into the kinetics of
the system and complicate the rate equation approach even more.

41
An example of this is the presence of a small amount of nitrogen.
Even in amounts of less than one part per million, spectroscopic anal¬
ysis of an alpha particle or fission fragment excited gas show the
presence of the first negative system of N+ with very intense band
z
peaks. This indicates the presence of an additional ion generating
term of significant magnitude to alter the population of many species.
N* is formed in several ways. The two most important transfer reac-
z
tions are
Hemetastable +
N„
He +
N2 +
e + AE
and
He2 +
N_
2He +
N2 +
AE
(35)
(36)
The Penning type ionization specified in reaction (35) is
normally considered the predominant reaction for the formulation of
the N+ ions. Thus the population of is predominately a function
3
of the population of the metastable He(2 s) state and the recombina¬
tion rate of N*. N+ will then increase as a function of increased
z z
helium gas pressure, since the collision rate, as well as the meta¬
stable population, also increases as a function of pressure. The reac¬
tion described in equation (36) also produces the N* ion, but at a
rate about five times slower than the Penning type ionization rate [43],
This is still significant, but the effect is diminished even more
because the population density of the molecular ion is far less than
the metastable state density.
The molecular helium ions are formed in many ways. The follow¬
ing reactions generate the majority of the ions.

42
He+ + 2He - He* + He (37)
O O
He(2 s) + He(2 s) - He* (38)
More information on formation and decay of these molecules is given
in References 43, 44, 45 and 46.
If the excited states are neglected and only number densities
of ion, atomic, and molecular species are included in the rate equa¬
tions, the set of equations is reasonable and easily solved with the
inclusion of only a few unknown reaction cross sections. Examples of
this technique, which include the effects of wall losses from the
excited gas, are given in References 26 and 47.
In order to study fission fragment-produced excitation without
using rate equations, it is advantageous to assume some model. Such
models, although probably invalid for exact representations, should
use an equilibrium distribution of excited states based on Maxwell-
Boltzmann statistics or some combination of equilibrium distribution,
plus a calculation of individual excited states by approximate cross
section.
The latter approach was used by Russell [16] in his calculations
of population inversions in argon. This model is presented here since
it is reasonably complete and takes into account most of the processes
for forming excited states in an individual manner, rather than by
empirical statistical distribution methods. It does ignore all
excited states other than those of atomic argon, and it would require
extensive modification to include analysis of ion excited states which
are experimentally available for study in fission fragment-generated

43
plasmas. Also, no provisions are made for inclusion of impurity species
in the equation set, but they could be added without great difficulty,
since most impurity interactions are loss terms for the primary gas.
This semiequilibrium model is similar in many ways to that used
by Leffert [47], except that in the latter case no attempt was made to
calculate excited states densities.
Using the theory of Bates, Kingston, and McWhirter [48],
the production terms for argon excitation have been reduced to five
principal processes:
1. Recombination of thermal electrons with atomic ions
2. Inelastic collisions between excited atoms and thermal
electrons
3. Radiative transitions
4. Direct excitation due to fission fragments and high
energy secondary electrons
5. Formation of excited states in the products of dissocia-
- * *
tive recombination of diatomic ions (He + e -* He + He ).
Ct
Combining the above processes, an infinite set of excited
state density functions are obtained.
CO
CO
q¿p
q co
+ n
e
q¿p
q>p
+ S.
(39)

44
where
n . . =
(P)
n =
e
n. =
(q)
K, ,
(P,c) =
K . . =
(p,q)
A(p,q)
G(p,q)
K(q,p)
A(q,p)
G(q.p)
K(c,p)
excited state number density, state p
electron number density
excited state number density, state q
inelastic cross section for collision of an excited
state with a thermal electron producing ionization
(loss term)
inelastic cross section for collision of an excited
state with an electron producing excitation from
p to q (loss term)
radiative transition rate for loss by a transition
from excited state p into q
correction term to account for optical trapping in
resonant transitions, transition from p to q
inelastic cross section for collision of a thermal
electron with the excited state q producing the
excited state p (gain)
radiative transition rate for gain by a transition
from excited state q into p
correction term to account for optical trapping in
resonant transitions, transition from q to p
cross section for 3-body recombination from continuum
to excited state p (gain)
radiative recombination cross section producing
excited state p (gain)

45
= source term for formation of excited states in the
process of dissociative recombination (gain, but
usually ignored).
S$ n T]i|r, . is a production term for excited states (p) due
a (p)
to direct excitation from fission fragments and the secondary electrons
they produce. ' This term is assumed constant throughout the volume in
question and is analogous to the production rate for atomic ions.
S§n = partial generation function that includes neutron
a
flux §, atomic number density n and a geometry
cl
term S
T] = ratio of total excitation rate to atomic ion produc¬
tion rate = 0.53 [24]
\lr . = ratio of the excitation cross section for array p
(P)
normalized with the cross section for the first
excited state (i.e. , for argon, the 4s array),
assuming
I
n=2
(P)
= 1.0
(40)
The cross section ratios can be calculated using the theory of
Gryzinski [49] for electron-atom interaction or by any other method.
If relative excitation cross sections were known from experimental
measurements, they also could be inserted at this point.
The argon ion density can be.represented as follows:

46
^ = Sí n - mn^ Ar+ - D ——
dt a a 1 .2
n A
a
“ ne I fne [K(c,p) + 9(p)l " n
P=1 ^
.K
(P) (P,c) ( ’
(41)
where
S$n = direct ionization source term from fission fragments
a
and secondary electrons
2a +
-mn Ar
a
= loss term by generation of the molecular ion Ar^
Ar
-D — = loss by diffusion from the volume of interest.
1 > ^
n A
a
The next three terms are, as described previously, loss by
3-body recombination, radiative recombination,
The molecular ion density equilibrium is
dAr,
dt
2 A +
mn Ar
a
Ar,
tv Ar n
D 2 e
- D.
2 a2
n A
a
(42)
where
2 +
mn Ar = 3-body collisional production term
-a Ar n = recombination loss term
D 2 e
Ar:
-D
2 a2
n A
a
= diffusion loss term.
The electron balance is
n = Ar+ + Ar^ ,
e z
(43)

47
d(— n kT ) m
2 e e e
— = 4 —- kn
dt me
a
8kT
(n q . + n q ) (T -T )
ran e ei a ea e a
+ _ + S$nQEc0 •
rec rad a Se
(44)
The first term on the right-hand side is the elastic collision energy
loss assuming a Maxwellian distribution of electron energy about the
electron temperature T .
e
q . = electron ion cross section
ei
q = electron atom cross section
ea
Q = gain in thermal electron energy from inelastic
rec
electron atom collisions
Q , = line and continuum radiation losses
rad
SSn^Eg^= energy source term from fission fragment interactions.
The time dependence of all the rate and equilibrium equations
presented is much faster than any change in the fission fragment source
term; therefore, steady state solutions can be obtained by setting the
time rate of change of Ar+, Art, n , T , and n. s to zero.
2 e e (p)
Equations (39), (41), (42), (43), and (44) are an infinite set;
in order to generate a solution an approximation is required. Since
there exists a level adjacent to the continuum that is in Saha equilib¬
rium. at the electron temperature, it can be assumed that all levels
above this are populated with a normal Maxwell-Boltzmann statistical
distribution of states. If the n. . set of equations is truncated at
(P)
this p level, a closed set is obtained. The obvious problem is what
level to truncate the excited staté population calculation. Russell

48
assumed equilibrium above the 6p level and solved a set of thirteen
simultaneous equations by computer methods. His solutions for Ar I
indicate the presence of inversions in the 5S-4p and 4d-5p transitions.
Although the capability of lasing these transitions has not been
determined, other transitions of Ar I have been made to lase.
In review, this chapter has shown how a fission fragment
deposits energy and how one could calculate this deposition in several
3
geometries. It has been shown that the He (n,p)T reaction products do
not deposit significant amounts of energy into the volume of a glow
3
discharge in 15 torr He . A model of the reaction kinetics of a fis¬
sion fragment-generated "plasma" has been presented in order to
describe the basic processes that occur in such an excited gas.

CHAPTER 3
PLASMA RESEARCH APPARATUS
3.1 Introduction
Since previous researchers [33,35] have been fraught with great
difficulties when attempting spectroscopic analysis of in-reactor
plasmas, it was imperative that certain basic design criteria, devel¬
oped as a result of this previous work, be applied to the construc¬
tion of this apparatus.
Most of the difficulties involved the transmission of the
spectrograph of the low level light produced by the fission fragment
plasma. The glow discharge experiments have adequate light output to
overcome these problems; therefore, design was optimized for the fis¬
sion fragment interaction experiments. The experimental chamber and
peripheral equipment were developed using the following criteria:
1. Chamber size must be large enough in average path length
to take full advantage of the energy available from the
average fission fragment.
235
2. U fissionable coatings should be maximized in area and
thicker than the mean free path of a fission fragment in
the coating.
3. Solid angle light availability to the optical system from
the plasma should be optimized.
49

50
4. Luminescent components such as quartz (light pipe) should
be eliminated from the optical path where subjected to
large neutron fluxes.
5. The experimental chamber should be located at the highest
flux position available in the reactor and should contain
only low thermal neutron cross section material (except
235
for TJ in the fission fragment plasma experiment).
6. A high light power spectrograph and extremely sensitive
photomultiplier -should be used instead of photographic
techniques.
7. The design should include the capability of using high
purity gases.
The above guidelines were followed, utilizing trade-offs where
necessary, and the resulting apparatus, as described in this chapter,
proved quite successful in providing excellent spectral data.
A detailed set of criteria for generating data of the quality needed
to determine cross sections is available in Reference 32.
3.2 Primary System
Several alternate methods of studying spectroscopically an
in-core plasmawere investigated and two basic solutions were identi¬
fied: (1) a small spectrograph installed next to the plasma, internal
to the reactor, providing a large solid angle light gathering capabil¬
ity, and (2) the optical transmission of light up a tube to a spectro¬
graph.

51
The second method was chosen as most practical. It employed
a stainless steel vacuum chamber 9 feet in length and 7/8 inch in
diameter, with a standard Ultek cross on top (Figures 3-1,3-2), where
the light is transmitted at right angles to the vertically positioned
spectrograph. Various experiments were inserted into the tube where
they were held at the bottom by gravity.
Emphasis was placed on the use of standard fittings, flanges,
and sizes. This allowed the replacement and storage of activated
9-foot tube sections, thereby allowing experimental procedures to con¬
tinue without waiting for an activated section to decay.
3.2.1 Plasma Region
The outer stainless steel vacuum jacket allows insertion of
both the glow discharge and fission fragment apparatus into the high
neutron flux region of the reactor. The glow discharge experiments
included study of three different types of cathodes, flat, brush, and
hollow. The insulating structures for the flat and brush cathodes
(Figure 3-3) consisted of an outer 2 feet by 40-mm O.D. Vycor tube
with the bottom beveled inward. The cathodes made continuity with the
outer shell by gravity contact on the bottom of the casing. The ring
anode was spaced from the cathode by a 35 mm by 5-inch Vycor tube.
Electrical connection to the anode was made by an insulated wire run¬
ning up the inside of the tube.
The hollow cathode structure was similar except a Vycor insert
was built to support the small cathode.

52
Figure 3-1 Reactor Mounting

53
GLOW DISCHARGE EXPERIMENT
FISSION FRAGMENT EXPERIMENT
Figure 3-2
Chamber Experimental Sections

RING
za udi
.. t
:
/
/////////A
BRUSH AND FLAT CATHODE
GLOW DISCHARGE
HOLLOW CATHODE GLOW
DISCHARGE
FISSION FRAGMENT
EXCITATION
Figure 3-3 Chamber Detail - Reactor Region
â– 30.5 cm

55
Removal of these structures to allow insertion of the next
assembly was a simple matter of turning the chamber upside down, and
sliding out the apparatus.
The fission fragment interaction assembly (P'igure 3-3) was
a 40 mm diameter, 3-foot-long Vycor tube with a 30.5 cm length inter-
235
nal coating of U„ 0 and an indentation at the 30.5 cm distance to
O O
support the anode. For comparison, a glow discharge was occasionally
started inside this assembly, using the vacuum chamber bottom as
a cathode.
3.2.2 Vacuum Chamber; Optical, Gas
and Electrical Feeds
All chamber parts were designed around "Ultek" 2-inch
flanged fittings in order to aid in replacement and modification.
The outer shell (Figure 3-1) consists of a 9-foot, 1-7/8 inch O.D.
by 0.065 inch thick No. 304 stainless steel tube with a heliarc-
welded plug on one end a standard 2-inch fitting heliarc-welded on
the other end.
Placed vertically on top of the long tube is the 2-inch
standard cross. Matched to the cross is electrical feed through on
one side for connection to the anode, gas feed on the top and a vinyl
sealed quartz window on the other side.
The optical system consists of a 500-mm focal length fused
quartz plano-convex lens held and focused vertically by three align¬
ment wires (Figure 3-1). A right angle front surface mirror is held
and aligned by a mount inserted into the center of the cross. The
vinyl seal quartz window allows light to escape from the chamber and

GRAPHITE SMCIIK (3) 11/?" OlHHTEt wtsxtt
CJi
a
Figure 3-4 University of Florida Training Reactor

57
be focused 2 feet to the side on the entrance slit of the spectrograph.
Thus, the plasma is viewed through the ring anode at a solid angle
-4
of 1.18 10 steradians, and focused by the lens on the spectro¬
graph entrance slit after passage through the exit window.
-6
The maximum vacuum attained by the system was 1 X 10 torr
and the maximum design pressure was 760 torr.
3.3 Uranium Coatings
3.3.1 Coating Requirements
One of the most important factors in the production of
a fission fragment interaction plasma is the fabrication of a suitable
uranium coating for the experimental chamber. Requirements for the
coating included the capability of deposition on the interior of a var¬
iety of cylindrical surfaces, such as Vycor and stainless steel.
Interior dimensions from 10 mm to 44 mm and lengths up to 3 feet were
encountered.
3.3.2 Coating Thickness
In order to maximize the source strength and thus the
number of fission fragments available, coatings were made thicker than
the range of a fission fragment in the source material. The range of
a fission fragment passing through U^Og, the final product of the
coating procedure, is calculated [41] as follows, with K and E from
Figures 3-5 and 3-6:
cm
(45)

58
O 5 10 15 20
DENSITY (g/cm3)
Figure 3-5 K as a Function of Density

KINETIC ENERGY OF PRODUCTS (MeV)
59
MASS NUMBER A
Figure 3-6 The Kinetic Energy of Fission Fragments as
a Function of Mass Number r38]

60
Density of U 0 =8.3 —^
O O O
cm
K for U„0o = 0.294
ü O
mg
(cm2) (Me\f/3
Maximum expected fission fragment kinetic energy = 97 MeV,
for mass = 95; therefore,
mg
R = 6.206
cm
2 •
mg
A coating thickness of 10 —=■ was considered adequate to
cm
account for some nonuniformity of application.
3.3.3 Review of Methods and Chemistry
There are several methods for producing coatings including
ion deposition, electroplating, powder distribution on a binder, and
coating and ignition.
For the purposes of the fission fragment interaction exper¬
imental work the most flexible and inexpensive technique, coating and
ignition, was chosen.
Much detailed work was done in this area at Los Alamos Scien¬
tific Laboratory around 1945 under the title of "Zapon Spreading
Techniques" [ 51].
The basic principle [52] of the Zapon spreading technique is
as follows: An alcoholic solution of the nitrate of the substance to
be deposited is mized with a dilute solution of Zapon lacquer in alco¬
hol, acetone, or Zapon thinner. The resulting solution is spread or
painted on the foil backing, allowed to dry, and then ignited to remove
organic substances and to convert the nitrate to oxide.

61
Many variations of this technique are possible, and it is
applicable to a wide variety of substances. The procedures used in
this project generally follow those suggested by this work.
Many alternate methods of placing coatings on surfaces were
evaluated, but the only successful results were obtained when many
thin coatings -were added in succession.
The requirements for a successful coat include a liquid that
can be deposited in thin layers, does not evaporate too quickly, and
includes a binder to transfer the fluid to a very viscous substance
upon evaporation of the solvents. The binder is necessary to prevent
an unequal distribution on the surface.
The Zapon spreading technique for uranium used ethyl alcohol
235
as a solvent for U °2^N°3^2 • 6H20 and added Zapon lacquer as a
binder for the uranyl nitrate salt upon evaporation of the ethyl
aleo hoi.
Zapon lacquer is not available, so a chemical substitution of
"Testors" butyrate dope containing methyl cellosolve and isobutyl
alcohol was used. Unfortunately, this lacquer forms a gel with ethyl
alcohol so n-butyl acetate was added to dissolve the lacquer.
235
A detailed description of the preparation, of uranium foils is
given below.
3.3.4 Chemical Procedures
The procedure for producing the coating solution, as
detailed in Figure 3-7, is variable depending upon the form of metal
available. The following procedure starts with highly enriched
uranium (93%) metal.

Figure 3-7 Chemical Procedures
Coating Solution
o
to

63
1. Dissolve the metal in concentrated nitric acid (HNO^).
2. Dry the solution on a hot plate with the temperature below
200°F in order to avoid hot spots and thus production of
any UO . The result is UO [NO ] • 6H 0, a bright yellow
Z Z o z z
powder.
235
3. For each 4 grams of U , add 20 ml ethyl alcohol, 20 ml
of butyl acetate, and 20 drops of butyrate dope.
4. Variations in the above mixtures are possible, but the pro¬
portions given seem to work well in the coating process.
3.3.5 Mechanical Coating Procedure
The art of producing a U 0 coating involves application of
O O
many thin coats in order to avoid flaking of material. The following
procedure is detailed in Figure 3-8.
1. a. Vycor base - Using a clean tube, flush with 6NaOH
and then with distilled water,
b. Metal base - Using a clean tube, flush with 6N HNO^
and then with distilled water.
2. Place the cylinder on a rotating horizontal mount.
3. While the cylinder is rotating, place a thin, even coat
of solution on the inside of the tube, using a coating
tool such as a camels hair brush or, for long tubes,
a tube swab mounted on a wooden dowel.
4. While the cylinder is rotating, dry the coating with air.

Figure 3-8 Mechanical Procedures
for Coating
Oí

65
5. Fire the coating using a Fischer burner or propane torch.
This will first oxidize the uranyl nitrate to brown-colored
UO and then at higher temperatures to black-colored U 0 .
2 3 8
The butyrate dope will evaporate and leave a residue of
less than 1 per cent.
2
6. Repeat until coating thickness is at least 10 mg/cm .
Forty coats were adequate for the Vycor substrate.
The resultant coatings appear as a black ceramic material with
a surface area much greater than that of a flat substrate. This is
due to the porosity of the ceramic coat and has likely aided greatly
in the deposition of larger amounts of fission fragment energy into
the surrounding gas.
235
Since U is radioactive and most samples contain traces of
other isotopes, care was taken to properly handle and contain the
chemicals involved in the coating procedure.
3.4 Support Systems
Acquisition of various data describing the effects occurring
in a plasma is dependent on the following support systems.
3.4.1 Reactor: Neutron Flux and Gamma Dose
The experimental chamber was designed to be inserted into
the University of Florida Training Reactor. As shown in Figure 3-4,
the UFTR is an Argonaut-type reactor licensed to operate at 100 kW.
The thermal neutron flux available.in this facility at 100 kW is shown
in Figure 3-9 as a function of distance from the bottom of the

66
o
CD
LO
I
X
ZD
O
en
Figure 3-9
Distribution of Thermal Neutron Flux
along Experimental Chamber

67
experimental chamber. These measurements were taken, using standard
gold foil dosimetry. In order to measure the thermal neutron flux
actually available to the plasma region, all foil irradiations were
done inside the stainless steel experimental chamber. At 100 kW the
11 2
average flux over the length of the glow discharge is 4.7 x10 n/cm -
11 2
sec, and, over'the fission fragment plasma, 3.8 x 10 n/cm -sec.
7
Gamma dose in this area at 100 kW is estimated to be 1.1 x10 R/hr
at equilibrium.
Reactor power data relate directly to the flux and are based
upon two calibrated compensated ion chambers placed near the core.
The experimental apparatus was placed in the 1-7/8 inch center verti¬
cal access port located between the two fuel regions. This is the
highest thermal flux region available in the reactor, but it is also
the highest reactivity worth region. This presented certain problems
which will be discussed in Section 3.4.5.
3.4.2 Electrical Systems
There are two systems involved in operation of the apparatus,
other than those pow'er supplies and leads involved in diagnostic equip¬
ment .
In order to supply a high voltage DC field to the chamber
when studying fission fragment interaction light amplification, a 10 mA
5 kV calibrated DC supply was used. For current measurements, the
power supply was floated with respect to ground on a 100 ohm resistor
across which was placed a Keithly DC microvoltmeter.

68
Electrical systems for operating the glow discharge were more
sophisticated because an arc in the chamber could destroy the contin¬
uity of the experimental procedure by altering the cathode surface.
Therefore, a sensing circuit was designed to monitor the voltage across
the glow discharge. Upon sensing the large negative transient when
the glow discharge changes from an abnormal glow to an arc, Figure 3-10,
an extra resistive load is switched into the series load chain in order
to quench the arc and return the system to a glow discharge. Although
the quenching system operated effectively, it was rarely needed, as
will be explained in Chapter 4.
Glow discharge I-V data were obtained either by two voltmeters,
one connected to read glow discharge voltage and another across a 2 ohm
calibrated resistor to measure current, or by direct connections to an
x-y plotter.
The glow discharge electrical source consisted of three series-
connected ultra-stable Lambda power supplies with both variable volt¬
age and variable load controls. This system allow'ed operation over
wide ranges of gas pressure and glow regions.
All of this equipment was installed in racks and operated
remotely on the floor of the reactor cell, since dose levels were too
high on the reactor top face to allow long term access by personnel.
3.4.3 Gas Filling Systems
Two different systems were used for filling the chamber.
One of the systems, designed for ultra pure gas filling and mass anal¬
ysis of filled chambers [31], was located remotely from the reactor

Figure 3—10 General Gas Discharge I—V Characteristic
CT5
to

70
building, and could only be used in the glow discharge experiments where
neutron activation of equipment was minimal. Its capabilities allowed
precision filling of gases with impurities of less than 1 part per
million, and bake-out of wall adhered impurities such as H^O. The min¬
imum chamber pressure that was reached during pumping and bakeout was
—6
1 X 10 torr, assuring the absence of substantial leaks in the system.
For the fission fragment interaction experiments, where the
Uo0 foil is highly activated, gas fill was done while the apparatus
O O
was mounted in the reactor. The gas filling system used in this case
consisted of a remotely situated two-stage vacuum pump, needle valve
mixing equipment and pressure indicating systems. Minimum pump pres-
-3
sure on the system was 1 x 10 torr, thus allowing an impurity source
5
of air, with a 1 atm fill of pure gas, of less than 1 part per 10 .
It was expected that the main impurity would be Ng and that this would
show up in the spectrographic analysis.
Since the above facility was not capable of ultra pure filling,
it was decided that commercial grade gases would be adequate for these
early experiments. The analysis of the argon and helium that was used
5
did, in fact, show impurities, mostly Ng, of less than 1 part per 10 .
All experimental work was done with the chamber sealed due to
safety regulation as will be described in Section 3.4.5.
3.4.4 Shielding
Two main purposes were served when the elaborate shielding
cave system was built.

71
First, the dose available from the center vertical port without
shielding would not allow reactor operation much above 1 kW, two orders
of magnitude below needed flux levels. Second, the ultra sensitive
photomultiplier used in diagnostics is sensitive to gamma and without
shielding the DC level and subsequent noise is intolerable.
The shielding system is diagramed in Figure 3-1 and shown in
Figure 3-11. The cave around the center vertical port consists of
lead filler rings surrounded by steel and lead blocks. Borated poly¬
ethylene blocks were used to moderate and absorb either fast or thermal
neutron flux transmitted up the access port.
A secondary lead cave was constructed around the photomulti¬
plier tube and constituted the light tight mounting case for the photo¬
multiplier as well as a container for the immediate electronics required
for its operation.
With this shielding, the DC shift from gamma sources was 7.5 mV
at 100 kW reactor power with a measurable spectrum line height as small
as 2.5 mV. After processing the signal, a noise component of about
1.1 mV overlaps the data.
3.4.5 Safety
Experimental procedures that involve insertion of absorbers
and unclad fuel into a high worth region of a reactor must also include
many safety considerations.
The center vertical access port, where the experimental work
was done, is located, as shown in Figure 3-4, between two fuel regions
in a graphite moderator. This area is considered a high reactivity

72
Figure 3-11 Chamber Mounting and Shielding Cave

73
worth region because it couples the two fuel regions together. Any
thermal neutron absorber inserted into this region affects the reactor
criticality situation much more than this same absorber placed, for
instance, in the thermal column, where the reflection of neutrons back
into fuel is minimal. The experimental apparatus is not an extremely
heavy absorbed, but its negative reactivity effect on the core was
large enough so that in certain circumstances, where heavy absorber
gases were used and where the tube was inserted to a greater depth
than normal, the reactor could either not achieve criticality or could
not run at high power due to the negative temperature coefficient of
reactivity.
This problem could be overcome only by allowing removal of
enough reactor control blade (neutron absorber) so that the decreased
absorption would overcome the negative reactivity of the experiment.
Initial control blade removal levels were limited by the reac¬
tor subcommittee of the University of Florida Radiation Control Com¬
mittee to less than 0.6 per cent positive reactivity insertion. With
a positive reactivity insertion of greater than 0.6 per cent, the
reactor is in a prompt critical excursion or critical on prompt neutrons
only and thus in an uncontrollable highly dangerous situation (pos¬
sible destruction of the core). But, due to the large negative reac¬
tivity presented by the experimental apparatus that would counter¬
balance positive reactivity, the reactor subcommittee allowed removal
of the control blades to a position corresponding to greater than 0.6
per cent positive reactivity when the following requirements were met:

74
1. The apparatus is absolutely fixed and cannot move.
This requirement was satisfied by proper placement of the
massive weight of the shielding cave which could not be moved without
deliberate actions.
2. The gas fill is fixed in pressure, less than one atmo¬
sphere, and will not be changed while the reactor is
critical.
This requirement was satisfied by sealing the chamber before
each run and by placing a relief valve at the fill valve to keep pres¬
sures greater than one atmosphere from entering the chamber.
The fission fragment interaction assembly somewhat eased the
negative reactivity problem due to the coating's addition of about
4 grams of fuel to the high reactivity worth region.
After many hours of high power irradiation, the glow discharge
experiments had an activity which gave surface dose rates of about
400 mR/hr. This decreased to about 100 mR/hr in a few days and was
deemed not much of a problem, especially since there was no loose con¬
tamination. The fission fragment interaction assembly contained a
large area of unclad fuel (coating); when removed from the reactor, the
dose rates at the tube surface were about 100 R/hr. Therefore, remote
handling of the apparatus by the reactor overhead crane and long term
storage in the water shield tank (see Figure 3-4) was necessary before
disassembly of the chamber. The internal components of the chamber,
especially the upper section, were heavily contaminated with mixed fis¬
sion products and had to be handled properly during disassembly.

75
The vacuum pump exhaust which contained various radioactive
41 40
gases, usually Ar from activated Ar , was connected to the
UFTR's air handling system for filtration, dillution, and disposal.
The problem of cooling the glow discharge was handled by the
same air handling system, which displaces about 12 CFM through the
center vertical port.
3.5 Data Acquisition Systems
I-V, reactor power, and spectroscopic data were taken during
experimental runs. Current and voltage measurement are an integral
part of the electrical supply system and were described in Section
3.4.2. Data on reactor power, and thus neutron flux, were obtained
from the reactor operating console, utilizing two compensated ion
chambers.
Spectroscopic data were obtained using a McPherson, 3/4 meter,
criss-cross, Czerny-Turner mount, scanning monochrometer with the
O
grating blazed for 3000 A and an EMI 9558 QB photomultiplier tube
mounted in the shield cave previously described. Since the lens does
not identically focus all wavelengths on the entrance slit, the system
was operated in a slightly defocused manner to allow for less precise
alignment of the optical system. The photomultiplier cathode was
operated at -1300 volts DC and its load was 1 megohm (plotter input).
A Moseley 7000A X-Y plotter was operated on X time base while the
spectrograph grating was driven at constant speed, thus giving the
spectral line structure as a function of wavelength. Noise problems

76
were minimized by the use of a low pass filter and by operating both
plotter and grating drive slowly enough to allow detailed plotting of
line shapes.
The system was grounded, using a 10-foot rod driven into earth
below the reactor. Braided copper strap was used for connections,
allowing no ground loops and using the stainless steel experimental
chamber as the main ground bus.
The following chapters will detail the use of the equipment
herein described and present results and analysis of the effects seen.

CHAPTER 4
ANALYSIS OF "iN-REACTOR" PLASMAS: FISSION
FRAGMENT GENERATED AND GLOW DISCHARGE
When referring to the photon output from the "in-reactor"
plasma, it can be assumed that the plasma is optically thin or that
there is very little absorption of photon energy by the gas. In order
to analyze the optical emissions and determine some characteristics of
the excited gas, some model is useful. Since it is presupposed that
the excited gas is in thermal nonequilibrium, the most valid model, as
previously stated, is a coupled set of interaction rate equations.
Without a complete set of cross section data for generation and decay
of excited states, this type of model is not useful. These data are
not available in complete form; therefore, the rate equation and com¬
bination type approaches [15] are by-passed in favor of a more easily
applied method, Boltzmann analysis.
The assumption that fission fragment excitation produces a gas
that is in thermal equilibrium, where the electron temperature and
distribution of excited states is defined by Fermi-Dirac or Boltzmann
statistics, is probably not valid. But, there are certain features of
this type of model that can prove useful in determining trends in the
excited state densities and in the search for a so-called "negative
temperature" or population inversion for pumping of a laser. The most
77

78
important feature of this model is the capability of describing the
plasma by an exponentially dependent factor analogous to the Boltzmann
temperature. Pressure-dependent plots of this factor and the excited
state densities from which it is derived are described in this chapter.
Also included is a review of all experimental fission fragment inter¬
action data generated by this research and an analysis of these data to
determine the characteristics of the generated plasmas. A review of
3 4
the experimental results of the He and He glow discharge reactor irra¬
diations is also included.
4.1 Experimental Procedure and Data Analysis:
Fission Fragment Interactions
The three gases bombarded with fission fragments—helium, argon
and carbon tetrafluoride—gave a luminous output that was easily mea¬
surable both for atomic spectral line peaks and for molecular band peaks.
Data were recorded by the methods described in Chapter 3. A typical
spectral sweep is shown in Figures 4-1 to 4-5 for helium at 100 torr
pressure. A second sweep is required with a different recorder sensi¬
tivity when the line or band intensity exceeds the plotter peak value
(Figure 4-1).
An interesting feature of these data is the significant back¬
ground produced by gamma interaction with the photomultiplier. This
background supplies the error in the spectral line intensity measurements.
The large amount of gamma shielding shown in the previous chapter reduced
this background to a tolerable level so that the measurement error on
the low level lines was acceptable. Other sources of error, such as
deviations in reactor operating power and changes in the nature of

79
3850 A -> 4410 A
J'*%. w *”*«• m«.U.
>,*°' «0M- <<*W
Figure 4-1 Helium Spectrum

80
/ — -tfUl
0Ur»k V«v
ále 4¿*U >•*
*â– * VL
ro *&••»
3336 A + 3967 A
^ itL/s
\L*
V. *
,|.\t<: iV/:
3967 A -> 461S
y¿iíf
Figure 4-2 Helium Spectrum

81
Hits 4^ 5iV7
US /*%« ,».** *Sa*cm l“*-> '»«•'/’-
U- SV Vc^ ->Oci
i
5247 A ->• 5877 A
I i*-
Figure 4-3 Helium Spectrum

82
5877 A 6506 A
i
,-ar*
1'J' . I "
.‘1
v /, rr
^V'
\>v
* '
â– V
â– J
6506 A
7136 A
Figure 4-4 Helium Spectrum
U~ Li.

°>4.
83
7136 A
7762 A
Figure 4-5 Helium Spectrum

84
the gas fill, were deemed insignificant in most cases and are noted
where applicable. Errors associated with the band height measurement
of CF^ and its reaction products cannot be established since the molec¬
ular dissociation and recombination of the various species present are
continuing kinetic processes reaching equilibrium in a long time
frame (about 3 hours).
At 100 KW reactor power, the error in the intensity is a con¬
stant factor equal to ± 1.125 mV divided by the appropriate calibration
factor for the wavelength of interest. This error (AI) is shown on the
linear intensity versus pressure plots. For the logarithmic calculation
of relative excited state densities, the error can be expressed as AF,
the standard error, where
and
Therefore,
and
AF
3f
ai
AI
(46)
(47)
(48)
(49)
This is the error indicated by the error bars on the
Boltzmann plots.
Calibration of the system was accomplished by using a tungsten
lamp calibrated by the National Bureau of Standards and a mockup of
the experimental system. All of the optical elements included in the

85
experimental apparatus were included in the calibration procedure.
To avoid both reflection and second-order errors in the continuum
measurements, stepwise filtration using calibrated dielectric cutoff
filters was applied to the light source. No reflection or second-order
O O
terms were observed over the calibration range, 3500A to 8500A. The
system response curve was folded into the spectral radiance curve and
the result normalized to the highest value. This resulted in a rela¬
tive response function which provides calibrated relative intensity data
when divided into the measured intensity of a line. For wavelengths
O
below 3500A, the cutoff value for reasonable accuracy using a tungsten
lamp, theoretical response curves were used. The theoretical response
calibrated line intensities were not used in the Boltzmann plots, thus
introducing no systematic error in these calculations. These low
wavelength data are given as a function of pressure and population
density where their intensity values are not compared to other line
intensities. Second-order output was observed for the large bands of
the Ng first negative system in helium and the OH 3064& system in argon.
O
Since the system response below 3000A is small, other second-order lines
or bands were not observed from the ultraviolet component of the spectral
output.
For the fission fragment work, the spectrometer entrance and
exit slits were set at 100 microns, providing a resolution of about
O O
0.5A with a dispersion of 16A per millimeter. With this resolution,
O
accurate separation of some of the argon lines such as 4332.0A and
O
4331.2A was not possible; therefore, for these few cases, individual
line intensities were estimated using the relative intensity ratio

86
data supplied in the MIT standard tables [53]. Line identification was
also based upon these tables and the atomic transition probabilities
were obtained from the NBS standard tables [54,55]. Molecular band
identification was based upon the tables of Pearse and Gaydon [56].
All measured intensity values are peak values and line widths are
approximately constant due to the low-temperature plasma and the rela¬
tively poor system resoltuion.
In order to process the large amounts of data obtained from the
spectral plots into intensity versus pressure, excited state versus
pressure, and Boltzmann plots, the data were placed in arrays on disc
storage of an IBM 1800 process and control computer. According to needs,
the data were called into the various plot or output routines from both
keyboard control and access programs. Most of the data plots in this
chapter and in the appendices were derived from this processing system.
4.2 Helium
Interactions of heavy charged particles with helium have been
studied extensively and the nature of these effects should be quali¬
tatively similar to the effects of high energy, highly charged fission
fragment interactions in helium.
The energy level structure of the helium atom, shown in
Figure 4-6, consists of singlet and triplet system states, both having
metastable states. Emission lines from levels above n=4 were not
viewed, due to wavelengths being out of reach of the experimental equip¬
ment and excited state populations not being large enough to provide
adequate photon intensity in spontaneous emission. Helium is the

Term value— 1/cm
Figure 4-6
Helium Excited States and Transitions
co
<1

88
simplest of the multielectron gases; therefore, analysis of reactions
in the gas is not difficult, especially when compared to analysis of
argon transitions.
4.2.1 Helium Kinetics and Spectral Analysis
Several basic kinetic excitation and transfer reactions
have been identified in the general literature as applicable to
high-pressure (> 1 torr) partial interactions.
Ionization and population of the excited states of the helium
atom are a result of several basic interactions:
1. Direct excitation,
*
fission fragment + He He (50)
2. Direct ionization and high energy secondary excitation,
fission fragment + He -* He+ + e (51)
e + He -• He + e (52)
3. Secondary ionization
e + He -* He+ + 2e . (53)
A very important excited state source is cascading from higher
excited states,
3|< *
He -• He + hv . (54)
The recombination of ionized helium,
He+ + e“ - He*, (55)
is a very slow process and for gas pressures greater than 1 torr,
competes poorly with the formation of the unstable helium molecule
and molecular ion. The major formation mechanism is 3-body condensation,
He+ + He + He - He* + He .
(56)

89
Since the formation potential of He+ (23.18 eV) is only 1.4 eV below
the lowest lying state of the helium ion, this formation is energet¬
ically probable.
Other major formation mechanisms are:
1. Metastable formation,
He + He He* + e , (57)
mm2
2. Hornbeck-Molner formation [57],
He* + 2He - He* + e" + He , (58)
where only excited states with matching potential participate.
The helium molecular ion loses energy to the helium system by
3-body recombination,
He* + He + e" - He* + He , (59)
and the unstable molecule loses energy by dissociation,
He* + He - He* + 2He , (60)
thus populating the excited states of the helium atom. Other loss
mechanisms which occur near one atmosphere are the product of heavy
molecular ions,
He* + 2He - He* + He , (61)
¿i O
and a chain effect,
He* + e“ + He - (He*) + He - He* + 2He* . (62)
u «J Z
The formation of molecular species is severely affected by the pressure
4f
(and thus, collision frequency) of the gas. As the pressure of the gas
increases, the formation rate for these processes increases greatly.

90
There have been several reports of helium molecular band
emission in particle (alpha and electron beam) produced high pressure
plasmas with impurities below 5 parts per million [58,59]. Because
the impurity fraction of N in the gas systems described in this
research is about 50 parts per million, the reactions between the
molecular ions and are predominant over the spontaneous emission
of the molecular helium [18]. In other words, the molecular band
output is quenched by the addition of only a small amount of nitrogen.
The molecular bands of helium are thus not observable in any of the
spectral plot data of this research. These quenching reactions are
obvious in their presence due to the tremendous N+ molecular band
O
output observed (for example, on the upper scan of Figure 4-1) at 3914A.
The formation of N+ is a function of the presence of the helium molec¬
ular ion and atom, with reactions as follows:
He+ + N2 - + He2 , (63)
He* + No "* No + 2He* + e” • (64)
z z z
At pressures below 1 torr, the N+ ion can be formed by charge transfer,
He+ + N2 - He + N+ + N . (65)
These reactions products were not found in this research.
The Penning-type reaction between metastable helium and N2
also produces a large fraction of the N+ ,
He + N0 “* N't + e + He , (66)
m 2 2
since the appearance potential of N2 is 15.5 eV, which is below
3 +
the metastable state (2 S) energy of 19.82 eV. The N2 molecular

91
2 + 2 +
bands observed are of the first negative system (B Z p, -* X E g).
Molecular nitrogen band structure is also observed from the second
3 3
positive system (C TT -* B tt) . A review of the more important kinetic
processes in a helium system with a large nitrogen impurity is given
in Reference 43.
The upper trace of Figure 4-3 and the lower trace of
Figure 4-1 show line structures that have been positively identified as
o o
the Paschen a and 8 lines of the He II ion, 4685.7A and 3203.1A,
respectively. The formation and subsequent spontaneous decay of these
excited states is of major importance in the description of the kinetic
processes of fission fragment excitation. The formulation of the molec¬
ular ion proceeds quickly at high pressures, effectively quenching the
He II species and removing a source for spontaneous emission. Thus, the
relatively large output from these lines indicates that the formation
rate of He II excited states is very large and that the steady state
O
population is also quite large. The excitation energy of the 4685.7A
O
upper excited state is 51.01 eV, and, for the 3203.1A transition, 52.24
eV, both extremely high for a plasma that has a low thermal level.
These lines are not visible in most helium plasmas and can only be seen
in high temperature spark discharges. The presence of these two lines
has been verified in several other heavy particle-produced plasma exper¬
iments referenced by E. W. Thomas [32].
The only other He II lines available in the spectral region
O
that the equipment encompasses are the Paschen y (2733A) and Bracket a
O O
(6560A) and 8 (5411A); but none of these were seen. The Bracket 8 at
6560Á may have been present, but cannot be identified due to the

92
O
presence of the hydrogen impurity a line at 6560A. Since the hydrogen
impurity system (o'.P.y) can be recognized and is extremely weak, the
probability of the appearance of the molecular rotational band sys¬
tem is extremely small; in fact, this "hydrogen second series" could
not be found.
In conclusion, the spectral output of the fission fragment¬
generated excitation in helium is qualitatively similar to that gener¬
ated by a glow discharge, except for the presence of the helium ion lines.
4.2.2. Line Intensity and Excited State Density
One indication of the kinetic processes occurring in a gas
system is the variation of particular species' populations as a func¬
tion of pressure. These variations can also be used as a tool in iden¬
tifying pressure-sensitive population inversions that may be available
for lasing. An example would be the simultaneous increase in a line
intensity from an upper state and a decrease in line intensity of the
transition from the lower state of the first transition. Such a tool
can only postulate the presence of an inversion and thus lasing, since
there are many other factors involved in the generation of laser
emission.
All of the measured relative line intensities and relative
excited state densities are plotted versus pressure and listed in
Appendix I. Excited state densities are calculated in a relative
fashion, assuming that deexcitation occurs only by spontaneous emission.
The emission of a line can be expressed as
I =
u l
hv
N
u
V
4rr
(67)

93
where
A .
ui
= transition probabilities [54]
h
= Planck's constant
VuX
= frequency of photon
N
u
= number density of atoms in the upper state of the line
I
= intensity of a line in units of energy per time.
If a
negligible fraction of ionization and an equilibrium
distribution
of excited, states are assumed, then a source term is
substituted for N
II
;>
HH
u
AuX gu
—— hv — N exp (-E /kT) (68)
4rr n , o u
(T)
where
N
o
= number density of neutrals
gu
= statistical weight of upper state, u
u
= upper state
£
= lower state
U(T)
= partition function of neutral atoms
kT
= thermal energy
E
u
= excitation energy of upper state.
This
expression for the population of and, thus, for line
intensity, depends upon the number density of neutrals and the thermal
electron temperature which is based on a Maxwell-Boltzmann distribution
of the energies of electrons in the gas. If it is assumed that the
excitation generation term of equation (68) is a constant, then a rela¬
tive measure of the excited state density, N , is (\I /A „g ).
u v ufu

94
This value will then reflect the effects of pressure, temperature and
collisional deexcitation on the population of the excited state u.
These calculations of excited state densities do not reflect
energy transfer mechanisms (i.e,, the Hornbeck-Molner molecular ion
formation) other than decay by spontaneous emission.
If these alternative processes are present, the intensity will
no longer reflect the relative population of the state or the energy
input to the excited state. This, though, serves as a tool for study
of the kinetics of the system, since the alternate collisional loss
channel will increase in effectiveness as the pressure increases, due
to increased collisional density. Conversely, assuming a constant
energy source term (excitation cross section), the population of the
excited state should increase. Of particular interest in helium is the
way the formation of the molecular species (equation (56)) affects the
relative population of the excited states while the fission fragment
source is constant. This will be discussed after a review of the
pressure-dependent energy deposition function in helium and argon.
There is an effect on emission from the cavity caused by
geometrical shielding. A small ring anode, 5 mm thick, used to apply
an axial field across the cavity, effectively removes from the spec¬
trograph' s view the portion of the cavity next to the foil surface.
Therefore, the calculation of energy deposition versus pressure shown
in Figure 2-5 is not entirely valid for this experimental core.
A similar set of calculated values is shown in Figure 4-7 where the
deposition of energy by fission fragments in the optically shielded
volume is removed from the calculation using equation (31).

ENERGY DEPOSITION (Mev/sec)
95
10 100 1000
PRESSURE (Torr)
Optically Viewed Energy Deposition in Helium
and Argon as a Function of Pressure
Figure 4-7

96
A comparison of these data to those in Figure 2-5 shows that
the viewed deposition of helium changes very little due to the surface
shielding, but the argon deposition is greatly altered. This is
because argon has a density ten times that of helium and, at high pres
sures, the range of a fission fragment in argon is less than the
diameter of the experimental tube. Thus, a large proportion of the
energy available is deposited in the shielded volume. The curves of
Figure 4-7 are probably not representative for the highest pressures
shown since diffusion terms are ignored and average fission fragment
ranges are assumed, but the trends of the curves are accurate.
Figure 4-8 is an overlay of the deposition calculation on
an intensity curve. The shape of the deposition curve is similar to
many of the helium intensity and excited state density curves. This
suggests that the intensity of helium lines and, thus, excited state
densities, are linear functions of pressure (or particle density)for
at least the lower pressure regions . If the Maxwell-Boltzmann sta¬
tistics of intensity (equation (68)) are assumed applicable and a con¬
stant source temperature is allowed, then both the line intensities
and population densities should increase as linear functions of pres¬
sure. With the linear portion of the pressure-dependent deposition
curve factored into the expression, a linear intensity response as
a function of pressure would again be assumed.
This hypothesis is generally valid, as shown in Figures 4-9
and 4-10, for most excited states and intensities up to a pressure of
200 torr. At this point both the population of states and intensity
decrease. As will be shown in the next section, there is an abrupt
decrease in the Boltzmann temperature at this same point;

RELATIVE INTENSITY
97
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ HELIUM HE I 5015*7
x HE I 4921 • 9
Figure 4-8
Helium Intensity and Energy
Deposition as a Function of
Pressure
Energy Deposition (MeV/cm'

LOG XI/gA
98
PRESSURE (TORR)
Figure 4-9
Relative Excited State Population
Density as a Function of Pressure

RELATIVE INTENSITY
20 40 100 200 400 1000
PRESSURE (torr)
Figure 4-10 Line Intensity versus
Pressure - Helium
>0 o o

100
The.decrease at 200 torr of helium intensity and all the
population densities indicates an increased formation of helium mole¬
cules and molecular ions. This effect can be expected in this pres¬
sure region [46], The decrease in intensity from the excited atom
states is due to the removal from cascade of the atom population
sources by quenching reactions (equations (63,64)) of the molecular
species, He+ and He , with N to form N*. Page 212 clearly shows
Ci £ £ Z
this effect, as the N* system band peaks increase in intensity almost
£
exponentially with increased pressure.
O
Figures 4-8 and 4-9 show a distinct deviation of the 4471.5A
3
transition of the 4d D state from the effects previously described.
This can be explained by an increase, as a function of pressure, of the
nonradiative three-body Hornbeck-Molner-type [57] collisional transfer
' 3
of equation (58). The excited state energy of the 4d D state, 23.73 eV,
closely matches the formation potential of He*, 23.18 eV; so the prob¬
ability of this process occurring is high. Decreased emission from
this state does not indicate a decreased population of the state but,
rather, an increase in the effectiveness of the channel of deexcitation,
due to increased collision density at higher pressures. Figure 4-9 also
3
shows a change in the direction of the slope of the 4d D state curve
at 200 torr pressure, again indicating a definite decrease in the popu¬
lation of this state due to the cascade source transfer of energy to N2,
as previously described.
Both the 4387.6& and 3964.7A transitions from the levels 5d
to 4p ^P°, respectively, show a large premature decrease in emission
starting at 100 torr. Both of these excited states have the potential,

101
24.04 eV and 23.74 eV to form He* by 3-body collisional transfer.
The delayed decrease for this formation may be a result of a pressure-
dependent threshold or a steep increase in the formation interaction
as a function of pressure. This pressure effect could be linked to a
higher excited state potential of these states than is required for
this process. But a more likely reason is that the Hornbeck-Molner
3-body collisional transfer is dependent on the square of the particle
density, while the spontaneous emission deexcitation channel depends
3
only on time. The 4d D state in which the greatest 3-body transfer
effect is seen has an excited state lifetime three times as long as
1 1 o _3
that of the 5d D and 4p D states (0.251 xlO sec); therefore, it
could be expected that the predominant loss mechanism of these states
is spontaneous emission at low pressure and 3-body collisional
deexcitation above 100 torr. The only other excited state of helium
that has the proper energy level to allow transfer by the Hornbeck-
1 °
Molner process is the 4d D state with 4921.9A transition and an excited
O
state energy of 23.202 eV. The 4921.9A line does not have an abnormal
pressure-dependent curve. This can be explained as a low-probability
interaction, since the excited state potential is only 0.022 eV above
the formation potential of He*. This is a very small excess available
energy and may not be adequate for this formation mechanism.
In conclusion, the population of the helium atom excited states
by fission fragments has a linear dependence on pressure and, thus,
energy deposition, up to 200 torr. At this pressure cascade sources
begin being channeled into the increased formation of the helium molec¬
ular ion and subsequent transfer of energy to the h'2 impurities. Also,

102
the increase as a function of pressure of the formation of He* by
Hornbeck-Molner 3-body collisional transfer from excited helium is
easily identifiable.
4.2.3. Boltzmann Plot Analysis
When nothing is known about a plasma, one of the first
things that is done is to make a Boltzmann plot of relative population
of states versus the excitation energy of the states. This method
serves as a tool in determining the nature of a plasma as well as
ascribing to it an approximate electron temperature that the plasma
would have if the excited state populations followed Maxwell-Boltzmann
statistics. The plot technique requires the transferring of the line
constants of equation (68) as follows, for one species only:
I
v
^u¿ he
"4tT X Ü
(T)
N
o
exp (-E /kT )
u e
(69)
I \
BUAui
he N
4ttU
(T)
exp (-E /kT )
u e
, r \ i i , r he n i r-50401 ^
los kx=log XoX+L—J Eu
(70)
(71)
Log [\I/g A .] is then plotted versus E for each line and the
u UÍ u
resulting slope of a least squares fit is (-5040/T ). Thus, T
e e
represents the Boltzmann temperature.
If the scatter about the fit line is large, the plasma deviates
from the Maxwellian model substantially and a temperature representa¬
tion becomes a less applicable describer. The temperature obtained

103
with the Boltzmann plot technique has to be defined as the temperature
which an electron gas having a Maxwellian distribution would have to
have in order to excite a gas so it can emit radiation in a certain
energy region (the region plotted in the Boltzmann plot) which is
comparable to the average of the radiation observed in the experiment.
The philosophy of such a comparison is analogous to the one used to
link color temperature to black body temperature. A correlation coef¬
ficient has been calculated for each least squares fit to the data in
order to assess how close the observed distribution (within the energy
range under question) is to a Maxwell-Boltzmann distribution. The
larger the value of Vc in the following expression the closer the
approach to a Maxwell-Boltzmann distribution.
n
V
c
£ (x.-x)(y.-z)
i=l 1
r n - 2
£ (x -x)
Li=l
n
£
i=l
(72)
If V = ±1 , the sum of the residuals will be equal to zero and every
c
point is exactly on the line.
A complete set of Boltzmann plots for all helium measurement
pressures is located in Appendix II.
A Boltzmann plot of an electron-generated glow discharge plasma
at 5.7 torr helium pressure is shown in Figure 4-11 to be quite similar
to the 50 torr helium fission fragment-generated plasma of Figure 4-12.
This indicates that the excitation of the atom species in both cases
is mostly due to electrons. The one great difference between the
plots is the pressure, differing by a factor of ten. The plot for

LGG(LAMBDA *I/G *A)
104
BOLTZMANN PLOT
SPECIES-HELIUM I
PRES■= 5»7 TGRR
GLOW DISCHARGE
BDLTZ• TEMP»- 5020»2 DEG- K
rge
Figure 4-11 Boltzmann Plot - Helium Glow Discha

LOG (LAMBDA ♦* I /G * A)
BOLTZMANN PLOT
SPECIES-HELIUM I
PRES•= 50 TGRR
BDLTZ• TEMP * = 3374•B DEG* K
4*0 +
Figure 4-12 Boltzmann Plot - Fission Fragment
Excited Helium

106
760 torr helium (Appendix II) is also similar in many respects to the
glow discharge plot. In other words, the distribution of states in
the fission-fragment excitation is not greatly different from that of
the low-current glow discharge. Both excitation sources, as expected,
produce a plasma that obviously does not have an ideal Maxwellian-
Boltzmann distribution of excited states.
3
In all of the plots, the 4d D state is underpopulated or
below the least squares fit line because of the 3-body interactions
3
discussed in the previous section. The 3d D state is also far below
the fit line. Since this state does not vary much in population from
3
25 to 760 torr, it is expected that,, the n F states, the cascade source
3
for the 3d D state, are also underpopulated to some extent. It is also
evident that in general the 3s and 4p “'"p0 states are slightly over-
populated.
The error bars are small for most of the states and would not
alter the general conclusions. The correlation coefficient plot
(Figure 4-13) shows that the actual least squares fit to the straight
line is never very good and V averages between 0.2 and 0.4. The
first point, 25 torr, seems to be an excellent fit, but is different
from the other Boltzmann temperature plots in that the 5d state is
missing due to its very low intensity. Thus, a fit to this first point
cannot be compared to the others.
Figure 4-13 shows clearly that the trend towards a more ordered
system of helium atom excitation—and thus a trend toward a more equi¬
librium distribution of excited states—is a logarithmic function of
pressure where
V = 0.13 log [P] .
c
(73)

CORRELATION COEFFICIENT
107
Figure 4-13 Pressure Dependence of the Boltzmann
Plot Correlation Coefficients - Helium

108
o
5500
5000
£ 4500
<
% 4000
UJ
I—
3500
3000
_Q (0.84)
(CORRELATION COEFFICIENT)
...---0(0.27)
u
(0.21)
a
,.o
(0.32 yry
(0.40)
(0.36)
l I I I I I
-I I I I—I 1 l.J.
20
50 100 200
PRESSURE (torr)
500
Figure 4-14 Boltzmann Temperature as
a Function of Pressure

109
This effect is not unexpected since, as the pressure increases, so does
the collision frequency and, thus, the thermalization rate of the high-
energy secondary electrons and other particles. This effect has been
noted by other authors and reviewed by McDaniel [60].
Over the pressure region investigated, the Boltzmann temper¬
ature ranged between 3400 and 4600°K. If the 25 torr point is neglected,
there is a decrease of 500°K between 100 and 200 torr. This is reflected
in the previous section, where an abrupt change in most of the excited
state density curves occurs at this same point. Since the correlation
coefficient does not exhibit any fluctuation at this point, this temper¬
ature drop can be considered a valid trend (Figure 4-14).
The question of how valid the Boltzmann temperature is cannot
be answered easily. The glow discharge value was 5020°K and, as the
pressure increased, the temperature generally decreased. This indicates
a valid trend where the electron temperature would be expected to
decrease as the collision rate increases and the distribution of states
becomes more Maxwellian. The increase in energy deposition as the
pressure increases (Figure 4-7) makes a quantitative dependence on
pressure estimation difficult. Bhattacharya et al. [28] have measured
an electron temperature of 600°K in a similar situation using micro-
wave techniques.
It is evident from the Boltzmann plots that a helium plasma
generated by fission fragments exhibits a trend toward equilibrium
with increased pressure as well as a drop in Boltzmann temperature.
Evidence of a poor fit to the least squares fit line representing tem¬
perature and an abrupt Boltzmann temperature shift at 200 torr pressure

110
indicate that this plasma is truly nonequilibrium and that a true
Maxwellian electron temperature does not exist. The intensity and
excited state density curves also exhibit an abrupt shift in slope
where the temperature drops. This has been attributed to pressure,
dependence of alternate kinetic loss channels (such as formation of
+ * +
He ) , and deexcitation by charge transfer to N , forming N . Further
¿i Á
information on an electron energy distribution will be developed in the
next section.
4.2.4 Field Amplification of Line Intensities
To support the detector work described in the next chapter
and to try to find more information about the electron density and
energy distribution in a fission fragment-produced plasma, a variable
D.C. field was applied across the plasma region.
The ion pair generation rate of the fission fragment source
can be approximated from the I-V characteristics. As the field across
the ionized region is increased from zero, a first plateau called the
ion chamber region is reached (Figure 3-10). In this region the field
supplies enough energy to the electrons to effectively allow collection
at the anode of all the electrons generated by external means. The
current thus measured can be related through geometrical terms to the
ion pair generation rate. If the distribution of electron energy is
again assumed Maxwellian, the current density to the electrodes can
be expressed as
j = j exp
es ep
(-eV /kT )
o e
(74)

Ill
where j is the electrode current density produced by the effect of
the voltage, V , across the electrodes, and j is the random electron
o ep
current density. Both currents assume a Maxwellian distribution of
electron energy described by T . This equation is valid only if Vq
does not affect the steady state conditions of the plasma.
By taking the natural log of each side, one obtains
eV
Sn j = 3 ~
es ep kT
(75)
Thus, the slope of a plot of this function will give the electron
temperature.
and
S
slope =
log i
V
o
e
2.302kT
e
(76)
T = e = 5.35 X 103 oK
e 2.302kS S
(77)
The I-V curves of the available data are given in Figure 4-15
where the electron temperature has been calculated from the slope of
the recombination region. The first portion, or logarithmic section,
of the I-V curve is the recombination region where the electric field
is adding little energy to the system. The curve reaches a knee where
essentially all of the electrons produced between electrodes migrate to
the anode. After this knee is a straight portion called the ion chamber
region. This is the limit of the plotted data, since the power supply
current limit was reached. With high field strengths, the proportional
region is reached where cascade ionization is produced by the electrons.

CURRENT (amps)
112
Figure 4-15 Current-Voltage Characteristics of
Fission Fragment Excited Helium

113
Figure 4-16 provides information on the effect of the field on
the plasma. It is evident that there is little amplification of light
output from the helium atom in the recombination region. This aids in
validating the use of equation (74), since one of its greatest restric¬
tions is on use where the field alters the population of excited levels
of the plasma. At the knee of the curve, amplification across the ion¬
ization chamber region becomes prominently displayed to the limits of
the measurement.
The temperatures found by this method are very perplexing since
they are in the millions of degrees Kelvin, while the Boltzmann plot
technique found temperatures up to only 5000°K. Transferring to terms
of eV per electron, the 50 torr plasma has an average electron energy
of 178 eV and the 760 torr plasma 655 eV. These results show a trend
that is opposite that of the Boltzmann plots, higher temperature with
higher pressure. This reverse trend occurs due to a hardening of the
spectrum due to increased collision density.
Only one explanation can be offered for the pressure of the
high temperatures: The plasma has a large group of electrons with
high energies. Since all field-affected plasmas have space charge
regions, it must be assumed that the electron current, the majority
carrier, is space charge limited to high-velocity, high-energy elec¬
trons through the recombination region. Thus, all current measurements
reflect only high-energy electrons until the saturation point is reached.
The gradual increase in current after the knee reflects the addition to
the current flow of the lower energy electrons. The current density val¬
ues for the two collection regions, though, are almost identical and

CURRENT (amps)
114
VOLTAGE
Figure 4-16 Line Amlification and Current as a
Function of Applied Voltage - 30.5 cm
Long Helium Cavity
INCREASE IN INTENSITY (percent)

115
will be assumed so in the calculations. A high energy component of the
electron energy distribution is not an unreasonable estimation since the
initial ionizing particle, the fission fragment, has an energy in the
tens of MeV and the primary electrons must also have high energies;
therefore, the source of high energy electrons for this plasma is quite
large.
The electron density of the plasma is found from the values at
the knee of the curve where
-n e v
e e
J = 4
and
j = current density
n = electron density
-19
e = 1.602 x 10 coulombs
v = drift velocity of electrons.
In helium for electrons with energies less than 10 eV.
5 E
v — 7.6 X 10 —— cm/sec [61] .
(78)
(79)
Table 4-1 summarizes the values of electron density and ion
pair generation rates found for three pressure values. The total
11 - 3
electron density averaged around 10 e /cm and is almost an order of
magnitude higher for the high pressure case, as is the energy input.
The ion generation rate for a plasma is
dn
dt
(80)

116
1. Pressure
TABLE 4-1. HELIUM DATA
50 torr
100 torr 760 torr
Helium
2. Saturation
Current (ma)
5.2
6. 2
5.2
3. Voltage
500
600
1200
4. Calculated
Energy (MeV/sec)
Deposition
5. Calculated Ion
Pair Generation
Rate (Ion pairs)
3
cm -sec
11 11 12
1.3x10 2.5x10 1.16X10 Fig. 2-5
1.41 xlO
13
2.65 XlO
13
1.25 XlO
14
w = 29.7
[62]
bottle
gas
6. Measured
Boltzmann
Temperature (°K)
7. E/p
mm Hg
1.34 XlO6 1.55 XlO6 4.93 XlO6
.328
.197
.052
8. Drift Velocity
of Electrons
(cm/sec)
2.49 XlO5 1.5 XlO5 3.95 XlO4 [61]
9. Recombination
Coefficient
O
a (cm /sec)
-9 -9 4. x10
4. 3 xlO 8.7 XlO
-9
-7
[46]
(5. XlO ) [63]
10. Measured Total
Electron
— O
Density (e /cm )
5.11 XlO10 1.01 XlO11 3.24 XlO11
11. Measured Ion
Pair Generation
Rate (Ion pairs)
13 13 4.2 xlO14
1.1 XlO 8. 9 XlO A
(5.3 xlO )
cm -sec

117
where
dn
dt
= rate of change of ion pair population
Q = pair source function
a = recombination coefficient
n = ion pair density.
Since the plasma is steady state and n+ = n , then
Q = cm .
e
(81)
This same ion pair generation rate has been calculated using the
energy deposition calculation of Chapter 2, Figure 2-5, and an
averaged ion pair generation energy of 29.7 for normal helium [62].
The agreement of the calculated and measured ion pair gener¬
ation rates (Table 4-1, items 4 and 10) is quite good and lends excel¬
lent support to the energy deposition calculations of Chapter 2.
Recent measurements in high pressure gases [63] have produced
-7
a recombination coefficient at 1 atmosphere of 5 X 10 . This wrould
16 3
alter the ion pair generation rate to 5.25 x 10 ion pairs/cm -sec.
This value is much above the calculated value and probably reflects
additional sources to the gas.
As noted in Figure 4-16, the light amplification caused by the
field in the ion chamber region is nearly a linear function of applied
O
voltage for the 5016A He I line at 50 torr. The threshold voltage for
As the pressure
F V/cm
amplification is 400 volts, or —— = 0.328 ——-—
’ P mm Hg
increases, the threshold voltage for amplification increases more
E
slowly than the pressure; therefore, the
value decreases. Thus,
as expected, the mobility of an electron decreases with increasing
pressure.

118
Since the detector concept offered in the next chapter is
dependent on light amplification, another point of interest is the
dependence of the light amplification voltage threshold on electron
density. From equation (78) it is evident that if the electron density,
derived directly from the fission fragment source, is decreased and the
field strength held constant, then the current points along the I-V
curve will also decrease, resulting in only a change in the slope of
the line without altering the threshold potential of light amplifica¬
tion. Linearity of the response of light amplification to electron
density is expected. Additional terms adding to the fission fragment
generation of ion pairs, such as gamma pair production, could alter the
linearity of the light amplification with respect to the fission frag¬
ment generation term and thus to reactor flux and power. This effect
is noted in Chapter 5 at reactor powers below 10 watts and is probably
due to the large gamma levels present in the reactor.
O
The amplification factor of the 5016A line for 50 torr helium
E E
where — = 0.4 is 0.29. For 100 torr helium, utilizing the same —
value, the amplification factor is 0.447. Taking into account the
twofold increase in pressure, the normalized amplification factor for
100 torr helium is 0.224. — of 0.4 could not be found for the 760 torr
pressure. Considering the nearness of these two values, the amplifica¬
tion factor is probably only a function of pressure and field strength.
Field-produced light amplification is sometimes called "Townsend ampli¬
fication” and the Townsend amplification coefficient for field-
intensified ionization is usually given as a function of — [64].
The above further supports the assumptions that the light amplifica¬
tion threshold does not shift and that the amplification does not change

119
as a function of electron density. Amplification is a linear function
of electron density for a fixed field strength. The amplification
threshold does, as previously noted, shift with pressure. More infor-
/
mation on these effects will be presented for argon irradiations, where
more complete data are available.
From the temperatures found by the Boltzmann plot and probe
techniques, an estimate of the electron energy distribution function
can be made. An assumption is made that the number of electrons asso¬
ciated with the lower temperatures found from the Boltzmann plot tech¬
niques are the total electron densities found from equation (78)
(Table 4-1), using the experimental drift velocity expressed by
equation (79). The electron density associated with the high temper¬
ature derived from probe analysis is a function of the temperature-
derived drift velocity, V = 0/kT/ (2 n m^) . Furthermore, the electron
densities are modified by the temperature-dependent pressure equation
P = nkT. This assumption is supported by the fact that the two elec¬
tron gases are noncommunicative, since the relaxation time of the
-12
electrons with respect to neutrals is 1.6 X 10 second and with
—8 11 — 3
respect to ions is 6 x 10 second (50 torr helium, 3 x 10 e /cm ).
Thus, recombination does not affect the thermalization of the elec¬
trons; only random collisional deexcitation has an effect on the
electrons.
Figure 4-17 includes normalized electron energy distributions
calculated from the data for 50, 100, and 760 torr helium. R. H. Lo
[65] has used a Monte Carlo calculational technique to obtain electron
energy distributions for high-energy alpha interactions with helium.

-1
â– 2
â– 3
â– 4
â– 5
â– 6
7
8
9
K
1
i
50 torr
100 torr
760 torr
CALCULATED
DISTRIBUTION
a PARTICLES
10
-2
7T
,0
X
10 * 10° 10' 10‘
ELECTRON ENERGY (eV)
10'
'igure 4-17
Electron Energy Distribution -
Fission Fragment Excited Helium

121
One of these plots is included in Figure 4-17; it is evident that the
calculated energy distribution and experimentally obtained distribution
are similar except at the high-energy end. This deviation is expected
since the production rate of high-energy electrons is a function of
particle type and energy. The fission fragment in all cases has. energy
and charge much larger than the alpha particles used in the calculation.
For a similar source flux, the energy deposition producing high-energy
electrons would be larger for the fission fragment. Variations in the
energy distribution show a smaller high-energy peak for increasing pres¬
sure, but the distribution also shifts to higher energies. This shift
is probably a result of decreased relaxation time for the high pressures
and is indicative of a hardening of the spectrum. The region between
the two peaks is uncertain in magnitude due to a lack of data. Inter¬
pretations of the Boltzmann plots other than a single line fit could
also alter this distribution.
In conclusion, field-modified fission fragment excitation has
produced values for electron density and indicated the validity of the
energy deposition calculations. Furthermore, the amplification has
been shown to be a linear function of electron density, and an elec¬
tron energy distribution derived from the experimental data has been
shown to be similar to a calculated energy distribution.
4.3 Argon Excitation by Fission Fragments
Argon has a more complicated excited state structure than
helium. Since the ionization potential of argon is 15.76 eV, 8.8 eV
lower than helium, the presence of a large spectrum of the ion species

122
can be expected in most excitation situations. Atomic argon has two
metastable states and a very large number of excited states available
in the low energy region. This, along with the availability of the
ion excited states, results in a very rich spectral output. Fortunately,
the majority of the At I lines are located in the red region and the
Ar II lines in the blue region, with a large gap between. This facil¬
itates identification of the spectral lines and allows separation of
effects on the two species when viewed in a grouped manner, as in
Section 5.2.
4.3.1 Argon Kinetics and Spectral Analysis
Since argon is a noble gas and in the same closed shell
category as helium, kinetic equations (50) through (62) apply directly
to argon and need not be repeated. Argon does differ from helium in
that the formation potential of Ar* is 15.06 eV, only 0.7 volts below
the atomic argon ionization potential. This results in a different
importance of some reactions and a totally different interaction mechan¬
ism for impurity species. An example is that the Hornbeck-Molner inter¬
action (equation (58)) has a low probability of occurrence because the
appearance potential of Art, is much higher than any of the excited
states observed in the spectral output. Also, the probability of the
formation of N* is very small since argon metastable energies are too
£j
low for Penning-type reactions and the Ar* ionization potential is
below that of N't, decreasing the probability of charge transfer reac-
tions to a negligible value.

123
In general, the argon ion and atom spectra are similar to the
spectrum of a normal glow discharge, althovigh the line widths are smaller
due to a lower temperature Doppler broadening. Figures 4-18 to 4-23
are examples of the spectra obtained with the fission fragment excita-
O O
tion into 150 torr argon. The sweep is from 2700A to 8338A and includes
lower sensitivity resweeps of out-of-range lines and band peaks.
Prominent in the spectra are the large spectral lines of Ar I above
O
6900A (20 lines identified) and the excellent Ar II spectra below
O
5000A (49 lines identified). Encouragingly present are the argon ion
laser lines 4371A, 4545A, 4579A, 4658A, 4727A and the normally high
° o
power line 4880A. The 5145A laser line was not found. Two Ar III lines
have been tentatively identified at 3480.6A and 3391.9A.
O
The predominant impurity is the (0,0) band of OH at 3064A
2 + 2
(A £ -*X TT). Since 5.09 eV is required to dissociate HOH and 4.05 eV
to excite OH to the A^S+ level, a total of 9.14 eV is required to
generate this system. The metastable states of argon at 11.55 eV and
11.72 eV are ideal sources for production by a nonradiative disso¬
ciative reaction. Therefore, it is most probable that the strong
emissions of the OH system are excited in the following manner:
Ar + HOH - H + 0H(A2E+) + Ar . (82)
m
The h'2 impurities can be produced in a similar fashion since
the second positive band excitation energy is about 11 eV, just below
the metastable levels. Thus,
3_.
Ar + N - Nn(C TT) + . Ar .
(83)

Figure 4-18 Argon Spectrum

125
4602 A + 5232 A
Figure 4-19 Argon Spectrum

126
5232 A + 5859 A
5859 A -* 6482 A
Figure 4-20 Argon Spectrum

127
Figure 4-21 Argon Spectrum

128
77/7 jU«* *>-"<**. 7.5^ ^
771.7 A -> 8338 A
7450 A -*â–  7653 A
Figure 4-22 Argon Spectrum

129
í9»°r>
A
Í9ítr p~*
4 r
f-'üm
C~°
xa J
/m****‘Í/p.
6900 A -> 6980 A
Figure 4-23 Argon Spectrum

130
Other bands tentatively identified show the presence of a small amount
of oxygen in the system. All identified species bands and lines are
listed in the pressure versus intensity curves, Appendix III.
A careful search for second-order and reflection spectra has
resulted in only one identification, the second-order OH system around
O
6150A. Since the first-order system is extremely large, the presence
of a very small amplitude (1/30) second-order in the high sensitivity
region of the optical system indicates that other second-order bands
and lines will be in the background.
Ar^ has been identified by many researchers using high-pressure
argon (greater than 200 torr) and mass spectroscopic techniques.
o
A continuum around 2300A shifting slightly to longer wavelengths for
higher pressures has been produced by Strickler and Arakawa [66] and
S. Dondes et al. [18] using alpha particle bombardment of argon. They
have attributed this emission to Ar2. For argon irradiation by fission
fragments above 450 torr this same continuum is evident around 2300&.
Its measured intensity is weak, but it could be considered having
a moderately high emission since the optical system sensitivity has been
estimated on a relative scale to be less than one-tenth of the maximum.
Argon molecular emissions are probable since alternate deexcitation
mechanisms such as charge transfer with impurities are improbable.
When comparing these Ar^ reactions to those of the helium molecules
the above authors have reported a relative insensitivity of this emission
to the addition of impurities. This further supports the premise that
the emission is from Ar , especially since this continuum is present
only above 450 torr and its intensity increases along with the normally

131
expected number density increase of Ar^ with increasing pressure.
The continuum is not present in the 4.8 torr glow discharge.
In conclusion, the spectrum of fission fragment-bombarded
argon is similar to that of a glow discharge produced in the same
experimental situation, except for the presence of a continuum in the
ultraviolet region attributable to Ar and the possible presence of
several lines of Ar III.
4.3.2 Line Intensity and Excited State Density
As noted in Section 4.2.2, a study of pressure-dependent
variations in excited state densities can yield information on possible
population inversions for lasing. Ar II excited state reactions are
not connected directly to impurity concentrations as in helium; there¬
fore, only cascade and collisional deexcitation losses are available.
Thus, the alternative loss mechanisms of radiative recombination and
molecular ion formation are uniformly applied to the Ar II. This means
that the relative excited state densities for Ar II are generally valid
over the pressure range studied.
Appendix III presents the pressure-dependent relative line
intensity and relative excited state density plots for argon, includ¬
ing intensity plots of the impurity band peaks. In general, no radical
deviations in line intensity or population density are observed.
A survey of the Ar II species indicates an increase to maximum
intensity of the lines at 100 torr with a general decrease thereafter
up to 760 torr. Ar I intensities reach a broad maximum around 250 torr.
The deposition curve of Figure 4-7 indicates a maximum at 100 torr with

132
a decrease thereafter. Figure 4-24 combines the deposition curve of
Figure 4-7 with the average intensity curves of the Ar I lines and
Ar II lines. It is evident that the Ar II species more closely follows
the calculated deposition. Ar II is usually not produced by particles
diffused from another region, but by the high-energy fission fragments
and primary or secondary electrons produced in the immediate region of
energy deposition. The deposition calculation of Chapter 2 ignores
diffusion from the primary deposition point. Thus, similarity between
these curves could be expected. Much lower energy electrons and
uncharged fission fragments can diffuse large distances and can produce
the excited states of Ar I. This could account for the variation in
Figure 4-24 for Ar I, which would be exhibiting excitation in the
optically viewed area not accounted for by the deposition calculation.
For pressures above 300 torr, the viewed deposition calculation is an
underestimate of both intensity curves.
The emissions from the OH and N2 molecules are similar in pres¬
sure dependence to Ar I, with the change of intensity from 25 torr to
the peak being twice that of Ar I. This indicates an increasing
metastable population for increasing pressure.
Table 4-2 lists the cascades found in Ar II for the spectral
lines identified. Unfortunately, the lower transitions of the normal
laser lines cannot be evaluated since the emissions are in the far
ultraviolet. An analysis of the excited state densities resulted in
the identification of four possible population inversions:
4 1/2 0
1. 3p ( D)4d F - 3724.52A
4 3 4 °
2. 3p ( P)5s P - 4156.09A

ARBITRARY UNITS
Ar I
t I 1 I I I I I 1 I I I L.
100 200 300 400 500 600, 700
PRESSURE (torr)
Figure 4-24 Intensity and Calculated Deposition (Viewed) as a Function
of Pressure
133

TABLE 4-2. IDENTIFIED CASCADES OF ARGON II
Upper State — Transition — Lower State
4 3
2 4 3
—*
2 o
4879.9 —3p4(3p)4s
2p
1. 3p ( P)5s
P -4103. 9 -3p ( P)4p
D
4 3
4
4228.2 — 3p ( P)4s
P
4 1
2
4 1
4072.0 — 3p ( D)4s
3p ( D)5s
D-4448. 9
4 1
/ 2
A 1
—►
. o
4035.5 — 3p ( D)4s
7 D
2.
- 3p ( D)4p D
4 3
9
4 1
, 2
-
4300.7 — 3p ( P)3d
F
3p ( D)4d
F -3724.5
4 3 :
? 9
4481.8 -3p ( P)3d
" D
4 3
3p ( P)5s
4P-4156.1
4 o
4 3
4
3‘ 4 3
— 3p4( P)4p
D -
4331.2 — 3p ( P)4s
P
3p ( P)4d
F -3582.4
4 3
4
-
3729.3 — 3p4(3p)4s
4
P
3p ( P)4d
P-3937.4
4 o
4 3
4
4- 4 3
— 3p ( P)4p
s -
3850.6 -3p ( P)4s
P
3p ( P)4d
P -3868. 5
4 3
4
—»
3928.6 — 3p ( P)4s
P
3p4(3p)4d
4
D -3780. 8
4 o
4348.1 — 3p4(3p)4s
4P
5' 4 3
—3p ( P)4p
D
4 3
4
3p ( P)4d
F -3588. 5
4013.9 — 3p ( P)3d
D
4 3
00
4 o
4806.0 —3p4(3P)4s
4P
6. 3p ( P)4d
D -3491.5 — 3p ( P)4p
p
4 3
4
4401.0 — 3p ( P)3d
7. 3p4(3p)4d
4 4 3
D -3491.2 — 3p ( P)4p
V-
4371.3 — 3p4(3P)3d
4d
8. 3p4(3p)4d
2p — 3307.2 — 3p4(3p)4p
V-
4657.9 — 3p4(3p)4s
2P
4 3
2 4 3
O
4545.1 — 3p4(3P)4s
2P
9. 3p ( P)4d
P -3293.6 — 3p ( P)4p
2P°
4 3
2
—♦
4764.9 — 3p ( P)4s
P

135
4 3 4 o
3. 3p ( P)4d D -* 3780.84A around 300 torr only
4 3 4 0
4. 3p ( P)4d D -• 3491.54A slight possibility.
The first two states have relative excited state densities
75 per cent above the lower states of the transitions, while only
a possible inversion occurs for the third case around 300 torr.
In the fourth case, the inversion is slight, with the lower state
values only 10 to 20 per cent below the upper state relative densities.
The other nine cataloged cascades have lower excited state densities
far in excess of the upper state values. No cascades were viewed in
Ar I. The calculated population inversions theorized by Russell [16]
cannot be checked, since his transition arrays are not available in
the spectral data.
There are several unusual variations in the intensity versus
pressure curves of Ar II, such as for 4965.1A and 4228.2&. These
variations probably indicate pressure-dependent changes in kinetic
processes related to the formation of molecular species.
In conclusion, several possible population inversions have been
identified in the Ar II species. Also, no large deviations of any of
the spectral data from the pressure versus intensity curves have been
observed.
4.3.3 Boltzmann Plot Analysis
The numerous lines of Ar I and Ar II provide a large number
of relative excited state densities to plot for Boltzmann analysis.
Unfortunately, the states occur in separated groups in Ar I and in a
concentrated region in Ar II, allowing only poor determination of

136
Boltzmann temperature. Figure 4-25 is a plot for 600 torr Ar I where
the calculated temperature is 14,059°K with a correlation coefficient
of 0.211. Figure 4-26 is a plot of Ar II with a temperature of 68,499°K
and a correlation coefficient of 0.192. These are representative of
the Boltzmann plots which are included in Appendix IV.
Figure 4-27 summarizes the dependence on pressure of both
the correlation coefficient and the Boltzmann temperature. Unstable
behavior is the prevalent characteristic at pressures below 400 torr.
The correlation coefficient shows that the fit of the Maxwellian dis¬
tribution is poor at low pressures and more closely approaches a good
fit above 400 torr. The spread of values around the fit line is also
an indicator that the plasma is not in equilibrium with a specific
temperature, but is essentially a cascade system.
As was characteristic in helium, the Boltzmann temperature of
both the Ar I and Ar II species decreases with increasing pressure.
The glow discharge plots at 4.7 torr show an Ar II temperature
(Figure 4-27) of 35,700°K, far below the fission fragment-excited cases.
The slope of the Ar I fit was positive, indicating a low temperature
and data that were difficult to fit. This evidence indicates that the
effective equilibrium temperature of the glow discharge, if one could
be accurately ascribed, is much lower than that of the fission fragment-
excited gas. This, of course, could not occur (considering the power
inputs to the two systems) if Boltzmann temperatures were a true indi¬
cation of the plasma characteristics. Instead, it must be assumed that
the fission fragment excitation produces an electron temperature or
energy distribution that is high and capable of exciting the states

LOG(LAMBDA-I/G-A)
137
BOLTZMANN PLOT
SPECIES - ARGON I
PRES•- BOO TDRR
BOLTZ• TEMP— 1405S-5 DEG- K
4
Figure 4-25 Eoltzmann Temperature Plot 600 torr Argon I

BOLTZMANN PLOT
SPECIES - ARGON II
PRES— BOO TDRR
BDLTZ• TEMP— 6B43B-3 DEG- K
Figure 4-26 Boltzmann Plot Argon II, 600 torr

o
PRESSURE (torr)
o
.08
.06
<_>
o
t—t
.04
al
ai
O
o
.02
¿-►glow discharge Ar II
Ar I
Ar II
glow discharge Ar I
—i i i■
©-►Ar I
20 V/cm
©-►Ar II
-®—
200 400 600
PRESSURE (torr)
Figure 4-27 Argon Temperature and Correlation Coefficient versus Pressure
139

140
observed in the Boltzmann analysis. A similar conclusion resulted from
the analysis of helium irradiations. An electron energy distribution
will be described in the next section.
A field of 20 V/cm was placed across the excited section and
a complete spectral trace taken. The Boltzmann plot analysis indicates
an identical temperature to the nonfield case for Ar I, but a much
elevated temperature of 110,000°K for Ar II. Both correlation coeffi¬
cients showed an improvement. Since, as will be detailed in the next
section, amplification is selective toward the Ar I states, the only
explanation that can be offered is that there was a selective amplifi¬
cation of several higher energy states. This could only aid any popu¬
lation inversion that is present. A survey of the excited state sensi-
ties of field-excited and nonfield-excited Ar II shows that the upper
4 1 / 2
excitation energy states are increased. The 3p ( D)4d F state,
previously identified as a possible inverted state, has increased in
O
number density while the lower state of the 3724.52A transition remains
4 3 4
constant. The 3p ( P)5s P state has also increased, while the last
two possible inverted states decreased in population density.
Although the temperature associated with the Ar I states
remained constant (the slope of the fit line) all excited state densi¬
ties increased uniformly due to the field amplification.
4.3.4 Field Amplification
The field amplification of argon is similar in all respects
to the effects seen on the helium plasmas described previously. A log¬
arithmic I-V characteristic with associated line amplification data is
given in Figure 4-28 for a pressure of 150 torr. As for helium

AMPLIFICATION
141
Figure 4-28 Amplification and Current versus
Applied Voltage - 150 torr Argon
CURRENT(amps) xlO

142
(Figure 4-16), the amplification of the lines and bands does not get
large until far into the recombination region, although amplification
does start at lower field strengths for argon than for helium.
Appendix V contains the I-V characteristics and amplification values
for all pressures measured. Amplification is plotted on a logarithmic
scale with straight line slopes resulting. This indicates that ampli¬
fication is directly proportional to current density and a logarithmic
function of field strength where
I = I eaE (84)
o
with
I = intensity
I = initial intensity
o
E = electric field strength (V/cm)
0- = amplification coefficient (cm/V)
is the general form of the amplification dependence, valid where
amplification is at least 4 per cent. The amplification value used
in the plots is of the form
A =
AI
I
I-I
o
"1
, aE
(e
-1) .
(85)
o o
a is then dependent on pressure and species of atom and is equal to
O'
Bn (A + 1)
E
(86)
where
(87)
The values of ot/P as a function of E/P are given in Figure 4-29.
Using equation (85) and Figure 4-29, the field amplification of Ar I

§ (cm/V-torr)
143
Figure 4-29
Amplification Coefficient versus
Argon

144
lines in a fission fragment-excited plasma can be calculated with
a maximum error of ± 10 per cent. The curve and set of equations for
amplification are similar to those used to find the electron ionization
coefficient for field intensified ionization [64]. The o//P values for
Ar II shown in Figure 4-29 are inconclusive since the amount of data
available is not adequate to produce a complete curve. It is expected
that the continuum of the Ar II curve for higher E/P values will over¬
lap the argon values for the first Townsend electron ionization ampli¬
fication coefficient.
Since the amplification of the impurity species is a function
of their concentration and excitation of Ar I, the amplification values
for these gases did not fit equation (84). Fortunately, the impurity
gases present do not affect the argon species, as noted in Section 4.3.1.
The variations of E^ (excitation energy) for Ar I had no correlation
with the small variations of the amplification of individual lines for
specific E/P values.
From the curves of Appendix V, it is evident that the amplifica¬
tion occurs in groups with the lower E value species (OH and N ) show-
u ^
ing greater amplification than the higher value species (Ar I, Ar II).
But there is no linear or regular dependence of field amplification
on E .
u
Table 4-3 details the values from the data for electron density,
ion pair generation rates, temperature, and other items calculated by
the identical method used for helium.. The electron densities range
10 — 3
around 10 e /cm with temperature values for the high energy group
collected electrons being around 5 x 10^ °K. From Figure 5-5 it is

TABLE 4-3. ARGON DATA
Pressure
25 torr
75 torr
150 torr
284 torr
450 torr
600 torr
760 torr
Argon
Saturation
Current (ma)
0. 55
1.1
1.95
1.85
3.25
0.28
3.1
A = 10.17 cm
Voltage
300
400
600
600
900
3000
900
Calculated
Energy
Deposition
(MeV/sec)
5.4 X1011
l.i xio12
1.4 XlO12
1.5 XlO12
1.5 XlO12
1.5 XlO12
1.5 XlO12
Fig. 2-5
Calculated
Ion Pair
6.5 X10
1.3 XlO14
1.7 XlO14
1.8 XlO14
1.8 XlO14
1.8 XlO14
1.8 XlO14
w = 26.7 3
Generation
vol = 310 cm
„ , .Ion Pr..
Rate (—- )
cm -sec
Boltzmann
Temperature
Arl (°K)
15,000
37,901
20,632
24,302
15,840
14,059
17,322
Boltzmann
Temperature
Aril (°K)
55,455
88,260
77,509
99,804
82,263
68,499
62,617
,V/cm
E/P ( —)
mm Hg
. 394
. 175
. 131
.0693
.0657
.164
.0388
Drift Vel.
of
3.3 xlO5
2.7 XlO5
2. 5 XlO5
2. 2 xlO5
2. 2 XlO5
2.7 xlO5
1. 8 XlO5
[601
Electrons
(cm/sec)
145

TABLE 4-3 (Continued)
Pressure 25 torr 75 torr 150 torr 284 torr 450 torr 600 torr 760 torr
10. Recombination
Coefficient
O' (cm^/sec)
8. xlO
-7
2. XlO
-6
3. XlO
-6
r* _ ry
4.4 x 10 5. XlO
5. XlO
-6
5. XlO
-6
11. Measured
Total
Electron
Density
(e /cm)
4.1 xlO9 1.0 XlO10 1.9 xlO10 2.1 XlO10 3.6 X IQ10 2.6 XlO10 4.2 xlQ10
12. Measured
Ion Pair
Generation
Rate 3
(#/cm -sec)
1.4 xlO13 2.0 xlO14 1.1 xlO15 1.9 xlO15 6.6 xlQ15 3.4 XlQ13 9.1 XlQ15
13. Boltzmann
Temperature,
Probe (°K)
2.4 xlO 3.7 xlO
5. 4 xlO
4.6 XlO
8. 2 XlO
22. XlO
11. XlO
Argon
[671
146

147
evident that both Ar I and Ar II show an amplification that is a linear
function of reactor power and thus electron density. All values asso¬
ciated with the 600 torr gas fill are deviant from average values since
this fill was measured (as far as I-V characteristics are concerned)
before contamination from wall adsorbed sources had entered the chamber.
This initial gas fill was considered ultra pure (less than 1 part per
million impurities). The most prevalent effect is the lower conductiv¬
ity of the plasma due to the lack of the more easily ionized species
and OH. Although ionized species of these impurities have little
effect on the kinetics of argon, they will change the shape of the
I-V characteristics by allowing more low energy electrons in the system.
These impurities will not affect the general results of this investi¬
gation.
The total electron density is calculated using equation (78)
and the drift velocity data of McDaniel [60]. The electron density
pressure dependence is given in Figure 4-30, where shown is an increase
with increased pressure that is identical to the increase in the high
energy electron group temperature shown on the same plot. These varia¬
tions with pressure indicate a hardened electron energy spectrum with
increased pressure, along with an elevation in the total electron density
due to increased energy deposition in the experimental cavity.
Ion pair generation rates were calculated from the electron
densities (equation (81)) using two different recombination coefficient
distributions. Figure 4-31 includes both the calculated ion pair gener¬
ation rates from equation (31) and the two measured value curves. These
two curves are given since there is much question about recombination

ELECTRON DENSITY (e"/cm
148
PRESSURE (torr)
Figure 4-30 Electron Density and Temperature
versus Pressure - Argon
TEMPERATURE (°K)

GENERATION RATE (1/cm -sec)
149
PRESSURE (torr)
Figure 4-31 Ion Pair Generation Rate as
a Function of Pressure - Argon

150
coefficient values at high pressures. The dashed line ion pair gener¬
ation rates are derived from the recombination rates of Dolgov et al.
[67]. These values may be too large since the same article lists helium
recombination rates that are very large compared to recent measurements
[63], The other measured curve was obtained by using a pressure inde¬
pendent recombination coefficient. This also is incorrect and produces
an underestimate of the ion pair generation rate at high pressures.
The actual values of ion pair generation are somewhere between these
two curves. A comparison of the measured values with the calculated
production rates shows that the latter is an overestimate at low pres¬
sures and an underestimate at high pressures. The three values are in
agreement within an order of magnitude from 25 torr to 300 torr. This
is reasonable agreement considering the unknowns and approximations in
both measured and calculated values of ion pair generation rate.
Following the method described in Section 4.2.4, normalized
electron energy distributions have been calculated for the pressure
data points of argon (Figures 4-32 and 4-33). As was characteristic
of helium, the relaxation time of electrons with respect to neutrals is
much less than ion interaction or recombination relaxation times. Thus,
the separate electron energy regions can be said to be noncommunicative.
At energies less than 10 eV, the distributions are similar regardless
of pressure, but, above 10 eV, there are variations in the distribution
functions. As previously noted from Figure 4-30, with increasing pres¬
sure there is a considerable increase in the number density of elec¬
trons with high energies or a general hardening of the spectrum. As
described by Figures 4-32 and 4-33, the high energy region peak becomes

ENERGY DISTRIBUTION (normalized)
151
10
10
10
10
10
10
10
10
10
10
10
10'3 10'2 lo"1 10° 101 102 103
ENERGY (eV)
Figure 4-32 Electron Energy Distribution - Argon

152
*
Figure 4-33 Electron Energy Distribution - Argon

153
more pronounced and widens toward higher energies with increased
pressure. This same trend was noted in the electron energy distri¬
bution of fission fragment-bombarded helium. Like helium, these
distributions are a combination of several Maxwellian distributions
and are not similar to a single Maxwellian or Dryvestain distribution.
Due to the presence of the argon ion temperature value, the distribu¬
tion is considered more accurate than those of helium and the region
of uncertain data has not been included.
In conclusion, the field-amplified intensity of Ar I has been
fitted to an exponential function with an amplification coefficient
(a) as a function of E/P, which is similar to the Townsend ionization
coefficient for field-intensified ionization by electrons. Data points
were insufficient to generate a complete coefficient function for Ar II.
10 - 3
Electron densities were found to be around 10 e /cm with the temper¬
ature of the high energy group electrons collected across the space
0
charge being around 5 x 10 °K. The calculated and measured ion pair
generation rates were in reasonable agreement below 300 torr. Also,
a pressure-dependent set of electron energy distribution functions
has been calculated from the data.
4.4 CF - Fission Fragment Interactions
Fission fragment interactions with carbon tetrafluoride have
been studied by Pagano [35] with the total photon output located in
the ultraviolet region and measured to be larger than for other gases
studied. Spectroscopic analysis was not successful. No other studies
of heavy particle excitation of this gas are known. Interest in CF^ is

154
based on its similarity as a fluoride gas to the uranium compound UF .
b
It is expected that the chemical kinetics of both gases are at least
similar, since both gases are extremely electronegative (excellent
electrical insulators with no dipole moment) and are symmetrical struc¬
tures.
Three gas pressures were studied, 100 torr, 760 torr and
5.5 torr. The 5.5 torr pressure was used only to generate a glow
discharge spectrum. This spectrum showed the expected ultraviolet
bands, with CF^ dominating (Figure 4-34). Also noted on the spectrum
plot is the nitrogen impurity system.
The 100 torr pressure fission fragment-produced excitation
O
was not unlike the glow discharge spectrum with a broad peak at 3000A,
but there were no identifiable band peaks. W. Brown [68] has recently
observed this same broad continuum with electron bombardment of CF^
at 10 atmospheres. In the reactor environment, this continuum shows
an unusual behavior that suggests a slow change in the chemical com¬
position of the gas. AS shown in Figure 4-35, the intensity of the
peak decreases exponentially with time, reaching an equilibrium in
about three hours. This reaction is completely reversible. The fol¬
lowing reactions are suggested [35]:
Formation of C F as the predominant yield
CF* - CF + F (88)
2CF3 - C2F4 + F2 <89)
or
CF4 - CF2 + F2
2CF,
- C F„
2 4
(90)
(91)

o o
Figure 4-34 Glow Discharge through 5.5 torr CF^ - 2000 A -* 5087 A
155

Figure 4-35 Band Peak Intensity of 100 torr CF^ as a Function of Time
156

157
or from the ionized and electronegative species
CF* + CF~ - C F + 2F . (92)
4 4 2 4 2
From the data it is evident that the formation of C F„ is
2 2
pressure-dependent and reaches a maximum around 100 torr. The reversing
of these reactions by interaction with F would account for the
decreased optical emission at higher pressures. This was also seen by
Pagano [35]. The further dissociation and reactions of into CF
and other species would-account for the decrease in the continuum out¬
put as the irradiation period continues. This implicates excited
O
as the source of the continuum centered around 3000A.
The irradiation of 760 torr CF^ produced an optical output that
included a distinct band structure on top of the continuum. This emis¬
sion is very pressure-dependent, since it was not observed at 100 torr.
These band peaks shown in Figure 4-36 cannot be identified as CF , CF,
F , or CF+, and they are totally different in wavelength than the
glow discharge peaks (Figure 4-34). Figure 4-37 shows a detail of
this spectrum where the periodicity of the structure is obvious.
Since the spectrally observed chemical changes seen at low pressures
are not significant at 760 torr, it is expected that this band system,
as detailed in Table 4-4, is representative of a molecular electronic
spectrum of CF^ with the vibrational system producing the individual
band separation. The system could also be representative of CF^ or
another gas produced by dissociation and recombination.
In conclusion, the presence of this new band structure for
high pressure CF^ lends support to the px-emise that there may be

o o
Figure 4-36 Spectrum of Fission Fragment Excited CF^, 760 torr - 2000 A -*â–  5087 A
158

o o
Figure 4-37 Spectrum of Fission Fragment Excited CF^, 760 torr - 2646 A -*â–  3280 A
â– 
159

160
population inversions in CF^ and perhaps in UF^ that have as yet to
be found and that can only be produced by particle excitation.
TABLE 4-4. CF^ FISSION FRAGMENT IRRADIATIONS;
4
BAND PEAKS OBSERVED AT 760 TORR
o
Band A
Spacing between
2848
18
2866
37
2903
55
2958
59
3017
56
3073
67
3140
67
3207
15
3222
4.5 Glow Discharge Irradiations
Studies of glow discharges were undertaken in order to find
the mechanisms for disturbance of the equilibrium of the system by
irradiation with a mixed reactor source of thermal neutrons and gamma
radiation. Previous research into the effects of reactor irradiation
of C02 lasers [11,13] has indicated a general improvement of efficiency
or, in effect, an improvement of the laser output. Those researchers
looking for alternative preionization sources for pulse lasers [69]

161
have found that the He (n,p)T reaction can be of help, along with
deposited fissioning foils, in decreasing the voltage required to
ignite the discharge. The purpose here, as described in Chapter 1,
is to understand the mechanisms by which the glow discharge is effected;
whether the effect is purely volume generated, cathode generated, or a
combination of the two. The response of these effects to various
cathode configurations was also studied.
4.5.1 Experimental Procedures
Three types of cathodes—brush, flat, and hollow—were
inserted into the experiment, as described in Chapter 3, and placed
in the center vertical port of the UFTR. For each cathode, various
gas mixtures were used. In each experimental run, both I-V character¬
istics and spectral lines were monitored. Also, for certain configura¬
tions, reactor shutdown and decay was followed. In several cases,
impurities were left in the gas in order to determine their effect on
the equilibrium under irradiation. In all cases the glow discharge
was operated at a fixed power level before data were taken, in order
to bring the temperature of the components to a steady state level.
Variations around this level were noted and are a result of changes in
both wall losses and the small thermionic emission component of cathode
electron emission.
4.5.2 The Glow Discharge
The various mechanisms involved in the maintenance of a
glow discharge are well understood and well documented in the general
literature. It has long been recognized that the most important portion

162
of a glow discharge is the cathode region; specifically, the cathode
dark space where the processes essential to the maintenance of the
discharge occur. This is evident in the fact that a glow discharge
can operate without a positive column. Thus, all external or internal
imbalance of a glow discharge must involve the balance equation for
the cathode region.
The current density balance equation for the normal glow
describes the basic effects, which consist of three groups,
.+
(j ) = y.j + f ,v n (j ) + f Y n (j )
e c Yi c d'p dec gYp g eg
(93)
where i+ is the ion current density at the cathode; f is the
c d
fraction of photons from the dark space which hit the cathode; and
n^ is the number of photons having hv>0 (the work function), produced
by primary and secondary electrons in the dark space. Equivalent to f^
and n , are f and n for the photons produced in the glow. The yield
a g g
coefficients for ions and protons are, respectively, y^ and y^, and
(jfi) is the electron current density in the glow regions.
From this equation it is evident that there are two main sources
of electron emission for the cathode, both related to the field strength
of the cathode fall. The sequence of balance in operation of the dis¬
charge first involves the emission of an electron from the cathode by
any one of the processes described above. This electron is accelerated
through the cathode fall where considerable kinetic energy is gained.
Through this region and beyond, the electron,and the secondaries it
produces,ionize and excite the gas, producing positive ions. These
ions are then accelerated through the field back to the cathode where

163
they produce further electron emission by positive ion bombardment.
This is expressed by the first term of equation (93). The field-
accelerated electrons and their secondaries continue exciting the gas,
dissipating the remainder of their energy into a region called the
negative glow, the region with the largest photon emission density in
the glow discharge. The photons from the negative glow produce photo¬
emission from the cathode surface, this being represented by the third
term of equation (93). The second source term is a result of ultra¬
violet photon emission from high excited states in the regions between
the negative glow and the cathode (Aston dark space, cathode glow,
cathode dark space). Other minor source terms that are not represented
in equation (93) and are still dependent on the cathode fall are
(1) thermionic emission from the cathode heated by positive ion bom¬
bardment, and (2) metastable Penning ionization processes (as in equa¬
tion (66)) in the cathode fall region. Several researchers [70] have
shown that the positive ion and photoemission processes are approx¬
imately similar in importance in the maintenance of the cathode emis¬
sion and that the photon contribution becomes increasingly important
in the abnormal glow region. This balance is dependent on the follow¬
ing items usually assumed constant for a particular operating discharge
1. Gas pressure
2. Gas type and impurities
3. Cathode material
4. Operating temperature (cooling capabilities).
The effects of these items on the cathode fall can be large and are
tabulated by many authors [64,70].

164
It is evident that any additional source term added to equa¬
tion (93) entirely independent of the current density or cathode fall
will affect the balance equation in such a way as either to increase
the current density for a constant cathode fall or reduce the cathode
fall for a constant current density. This additional source term and
its effect with several gas types and cathode configurations is the
topic of the next three sections.
4.5.3 General Reactor Mixed Radiation Effects
on the Glow Discharge
The trend of radiation effects on all of the glow discharge
situations studied was a decrease in the starting and maintenance
voltage and current required. This decrease in the I-V character¬
istics slowly disappeared as the current and voltage were increased
into the abnormal glow region. Absent in many cases was the region
called the subnormal glow discharge.
3
The I-V characteristics of a He -CO^-Ng, 8:1:1 mixture glow
discharge are shown in Figure 4-38 for several cathode configurations.
The reactor effects shown by these curves are typical of the effects
3 4 4
viewed using the three cathodes with He , He , and He -CO^-Ng gas
fills. The brush cathode was found to be unsuitable for most exper¬
imental situations due to its many step voltage levels, a function of
the construction of the cathode. Therefore, use of this cathode was
discontinued after early experimental procedures. The hollow cathode
shows the greatest reactor effect with its surface area being larger
than the flat cathode. The two-level curves are typical of hollow
cathode glow discharges with large amounts of present.

Figure 4-38 Glow Discharge I-V Characteristics for He - CO^ “ N2 * 10 torr
165

166
The I-V characteristics for several gases using a hollow cathode
are detailed in Figure 4-39. It is evident that the presence of low
ionization potential gases such as has a much larger effect on the
3
glow than does the presence of He . Since the scale used in this
3 4
plot is large, the differences in the He and He curves are small;
therefore, only one characteristic is shown for the two gases.
The largest variation in an I-V characteristic from reactor
radiation was for N at 3.3 torr using a flat cathode. Figure 4-40
shows these data where the normal I-V curve has a typical glow dis¬
charge shape and the irradiated glow curve has decreased as much as
130 volts for low currents.
The downward slope of the I-V characteristics of the N2 mixture
shown in Figure 4-39 is a result of thermionic emission from the low-
mass hollow cathode. The N* bombardment of the cathode generates much
heat, which is not dissipated efficiently.
In order to further delineate between the effects of the
3
He (n,p)T reaction, gamma photoionization, and gamma photoemission,
data were obtained on the decay or change of the glow discharge voltage
with constant current when the reactor is "scrammed’' or shut down
quickly. This scram procedure results in a known decrease of neutron
flux along with a much slower decrease in gamma radiation. Figures 4-41
and 4-42 give the decay curves of glow voltage for constant current for
several gases on hollow and flat cathodes. These curves are normalized
to initial voltages and expressed in terms of fractional change.
Although the variations in these curves are small fractions, they rep¬
resent large changes in current if the voltage is held constant.

900
800
700
600
500
10 20 30 40 50
CURRENT (ma)
rigure 4-39
I-V Characteristics for Hollow Cathode Glow Discharges
167

VOLTAGE
800 r
600 1 1 1 1 1 L
0 10 20 30 40 50 60
CURRENT (ma)
Figure 4-40 I-V Characteristics, 3.3 torr Glow Discharge, Flat Cathode
168

10.5 torr
10 torr
10 torr
TIME (min)
Figure 4-41 Voltage Decay, Glow Discharge, for Reactor Shutdown - Constant I, 20 ma
169

170
LU
O
c
Ic
o
LU
CD
<
<
O
o
c
or
TIME (min)
Figure 4-42 Voltage Decay, Glow Discharge, for
Reactor Shutdown - Hollow Cathode

171
Two effects are noticeable on the decay curves. First, the
effect of the reactor is far greater on the hollow cathode and much
greater on gases (or mixtures) that include low ionization potential
3
components such as N2* The effect of the He (n,p)T reaction is also
4
clearly shown in comparison to irradiation of He which exhibits only
gamma effects.
Other data have shown that the effect of the reactor on the glow
discharge is a linear function of reactor power (each power point com¬
ing into temperature and gamma equilibrium) with the amplitude of the
effect being a function of the slope of the I-V characteristic envelope
for the reactor powers measured. This is especially evident in a con¬
stant voltage versus reactor power measurement using N2 and a hollow
cathode. The current actually decreases for increasing reactor power
while following its I-V characteristic.
The next two sections will discuss the source of the glow
discharge variations relating to equation (93) and the mechanisms for
the effect of the gamma and neutron components of the reactor radiation
source.
4.5.4 Volume Deposition
There are two specific methods by which volume deposition
can affect the optical and electrical characteristics of a glow discharge.
If the deposition is uniformly distributed across the glow, there
will be additional excitation in the positive column, enhancing the
spectral output of the plasma. A second perturbing volume deposition
source is the additional ionization produced by the external source in
the cathode fall region. Ionization in the positive column will have

172
little effect on the total system when compared to the equal amount in
the cathode fall which generates an additional source term to equa¬
tion (93). Two volume deposition sources are available in this exper-
3
imental analysis, the He (n,p)T reaction and photodeposition from
reactor gamma. In Section 2»2 a calculation of the deposition of the
3
He (n,p)T reaction shows that this source is only a very small percent¬
age of the total power deposited in the positive column, especially
11 2
writh the available neutron flux of 3.8 x 10 n/cm -sec. At pressures
less than 15 torr, the gamma contribution is also extremely small.
There is a possibility of viewing the excitation and ionization changes
produced in the glow discharge by these sources if the measuring equip¬
ment is sensitive enough to see these small changes. In all cases there
was no reactor effect on any helium, helium impurity, N^, or CO^ line
or band for all mixtures at all measured pressures as long as the cur¬
rent through the discharge was held constant. Thus, it can be assumed
that, according to spectroscopic measurements, volume deposition sup¬
plies no additive effect on the spectral output independent of the
glow discharge.
The volume effect on the cathode fall region can be calculated
in an approximate manner from the energy deposition calculation of
Chapter 2. If a w value of 29.6 eV/ion pair is assumed, the ion pair
11 3
production rate corresponding to the 1.28 x 10 eV/cm -sec deposition
3 i 9
rate in 15 torr helium from the He (n,p)T reaction would be 4.32 x 10
3
ion pairs, cm -sec. This electron generation density is then subject
to amplification by acceleration of the original electrons across the
cathode fall, thus producing a net additional current density.

173
The calculation of the added current density is based upon a
15 torr helium glow discharge operating with a hollow cathode with
a current flow of 3 ma. The cathode has a plating of pure iron with
an effective area of 12.56 cm. The normal cathode fall for helium with
an iron cathode is 150 volts over a distance of 1.3 cm-torr or 0.0867 cm
[64]. The average field strength is 1731 V/cm with E/P = 115.2. For
this E/P, a/P, the first Townsend ionization amplification coefficient,
is equal to 2.1 ion pairs/cm-torr or a - 31.5. The effective electron
current density produced in a field by amplification of the internally-
generated electron density j is
J = 3 e
x o
ax
(94)
For an average value over the total fall distance d,
Jd = ( -19
where q is found from equation (81) and e = 1.6 x 10 coulombs/ion
—8 2
pair; j was found to be 1.06 x 10 amps/cm while the current density
-4 2
of the experimental glow discharge is 2.39 x 10 amps/'cm . A compar¬
ison of these two values shows that volume ionization supplies an almost
negligible source to the cathode equilibrium. This cannot be verified
by the experimental data available.
In conclusion, it is evident that for reactor powers below 100 kW
11 2 3
(neutron flux less than 3.8 x 10 n/cm -sec), the reaction He (n,p)T
and gamma sources do not contribute any effect by volume deposition in
low pressure glow discharges other than a small preionization that aids
in starting the glow discharge.

174
4.5.5 Cathode Deposition
Two external sources are available from the reactor for
irradiation of the cathode: (1) gamma for generating photoemission
3
electron sources and for the gas loads including He , and (2) the
thermal neutron reaction generating energetic protons and tritons for
heavy particle-produced electron ejection. It must be emphasized that
these two sources are similar to two already existing electron source
terms, positive ion bombardment (the first term of equation (93)) and
photoemission (the last -two terms of the equation).
It has been previously established that both gamma and the
3
He (n,p)T reactions are effective in altering the characteristics of
a glow discharge; according to the results of the previous section,
the effect is not from volume deposition. Thus two extra terms are
added to equation (93), suggesting that all effects are a function of
cathode emission.
.+
(j ) = y. j' + f y n (j ) + f y n (j ) + y 0 + Y-0 (96)
e c Yi c d'p dec gYp g e g Tp y 1 P
where
0 = gamma source to the cathode surface
Y
Y = photoelectric yield as a function of quantum energy
P
0 = particle flux source to the cathode
P
y = electron yields from particle bombardment.
It has been established that for constant (j ) the internal photon
e c
emission from the glow remains constant (constant photon source terms);
therefore, the effect of the added last two electron current source
terms must be to decrease the value of j+. Since the energy and, thus,
c

175
Y
electron ejection capability of the positive ions is directly propor¬
tional to the cathode fall, the experimental evidence of the linearity
of the drop on cathode fall with respect to an increase in the terms 0
and 0 indicates that the source term of j+ does decrease,
p c
The large changes in the glow discharge under irradiation,
caused by the addition of N , could be a result of additional ion pair
production terms from Penning ionization of N by the helium raetastables.
z
A more likely cause would be the increased cathode fall (150 volts for
He to 290 volts for N ) and decreased fall distance, providing an
z
increase factor in the fall region field strength of about 4 for iden-
4
tical gas fill pressures of He and N . Thus this increased field
z
strength for identical pressure fills and operating characteristics
can only mean far more efficient use of the external source electrons
emitted from the cathode. This would increase the reactor effect on
pure N over pure He by a factor of at least 4. The data of Figures
4-41 and 4-42 verify this conclusion.
The current source at the cathode, from the external source
terms, can be approximated using the typical glow discharge described
3
in Section 4.5.3. For a 15 torr fill of He the reaction, or source,
11 2
rate of protons and tritons in a flux of 3.8 x 10 n/cm -sec is
9 3 3
1.076 x 10 reactions/cm -sec. An approximate volume of 70 cm is
3
available for a total deposition source of particles (50 cm internal
3 11
plus 20 cm external), thus the bombardment rate is 1.51 x 10 par¬
ticles/sec.
-3
With a yield value of 10 [61], an electron emission rate over
2 11 2
the 12.56 cm area cathode would be 6 x 10 electrons/cm , or a current

176
-7 2
of about 1 x 10 amps/cm . These electrons have energies far above
those emitted by normal positive ion impact; thus, their effect in
altering the cathode balance is large. Assuming equation (94) is
valid and assuming a constant cathode fall, then the effective current
produced by low-energy electrons across the fall would be 1.54 x 10 6
2
amps/cm . If only a factor of ten is added to the multiplication due
3
to the high energies of these electrons, the He (n,p)T reaction-
produced current, y^0^, would be 10 per cent of the total glow current
and of considerable importance in the balance equation.
7
The gamma dose at 100 kW was estimated at 1.1 X 10 R/hr.
For 1 MeV average energy this would be equal to approximately
14 2
4.0 x 10 y/cm -sec on the surface. Assuming a quantum yield of
-3 11-2
10 , the net electron emission from the surface is 4 x 10 e /cm -sec,
-6 2
producing a net electron flux of 1.03 x 10 amps/cm . Although the
3
y effect is lower (than the ion bombardment effect of He (n,p)T) for this
helium glow discharge (as verified in Figure 4-42) it still produces a
significant fraction of the cathode current.
With external sources available, it is evident that a glow
discharge can operate with current densities and voltage drops much
lower than can unradiated discharges. I-V characteristic data such as in
Figure 4-40 verify this observation where a 17 per cent lowering of the
total input energy was obtained for a current of 6 ma. Even greater
reductions were observed in other data.
In conclusion, the reactor mixed radiation effect on glow
discharges is due to gamma photoemission from the cathode surface and
3
is a function of the ionization potential of the gas. Where He is

177
present, the reaction products bombard the cathode and produce a signif-
3
icant addition to the total cathode emission. In He the particle cur¬
rent source term is greater than the gamma photoemission source. For
3
mixtures of He and N , the effect of the particle-produced source is
decreased considerably and the gamma photoemission source predominates.
Glow discharges are able to operate at much lower input powers.
This will allow a lower gas temperature in the positive column and,
thus, a better matching of the temperature distribution to the optimum
value for CO^ Sas lasers. This has already been verified [13], The use
of particle and gamma sources for preionization of pulsed gas lasers
and irradiation of the cathode can result in considerable increase in
C0o laser output.

CHAPTER 5
APPLICATIONS OF FISSION FRAGMENT-PRODUCED PLASMAS
Upon preliminary review of the spectroscopic data obtained
from the fission fragment-produced argon plasma, it was evident that
enough excitation was probably available to produce population inver¬
sions in the argon II ion. Some of the original threshold density
15 . 2
calculations specified a minimum thermal neutron flux of 10 n/cm -
sec for lasing; but, due to the unusually high population of the
higher excited levels, it was felt that even with the low flux avail-
11 2
able (3 x 10 n/cm -sec), there might be a chance of lasing the
argon II ion.
Dr. E. E. Carroll [36] at the same time suggested a very novel
use of the Townsend amplification process seen in the plasma. Almost
all detectors that have been proposed for the liquid metal fast
breeder reactor suffer severe damage due to the high temperature and
high gamma levels, measuring the light variations in the plasma formed
in the reactor from a remote position seemed an excellent remedy for
the problem. The fission fragment plasma chamber was almost identical
to such a proposed device; therefore, the only modification made to
the experiment was in the method of processing spectral data.
178

179
5.1 The Nucíear-Pumped Laser
235
The design of a nuclear-pumped laser utilizing a U~ foil must
originate with the fact that once the foil is inserted into the reactor
and irradiated for a short length of time at high power, it can no
longer be easily handled due to the extremely high gamma radiation
being emitted from the fission products. Since the UFTR (Figure 3-4)
does not have a through port, the laser was designed so that the device
could be self-supporting, prealigned, and inserted into one of the
9-foot test chambers used for previous studies.
The data presented in the previous chapter do not give absolute
proof of population inversions, so it was necessary to encompass in
the cavity design a wide band of wave lengths in the blue region in
order not to miss some possible inversions. It was expected that the
o o
laser output would be at 4880 A and 5340 A, the usual high power argon
ion laser lines. A calculation of possible power output from the
laser can be made, assuming a 1 per cent conversion efficiency of the
energy deposited in the cavity. Following the theory presented in
11 2
Chapter 2, a neutron flux of 3 x 10 n/cm -sec will give a total
9 2
energy deposition in argon of about 3 x 10 MeV/cm -sec at a gas
pressure of 150 torr. The cylindrical foil has a diameter of 1 cm
and a length of 91 cm; therefore, if the total volume could be swept
by the laser cavity, and an efficiency of 1 per cent assumed, a power
output of 1.37 milliwatts would be seen. For a realistic optical
cavity of about 1 mm in diameter, a power output of 13.7 microwatts
would be transmitted out of the cavity. This is an exceedingly small

180
output, but under the correct conditions this photon output could be
observed and measured for coherence and spectral content. Three
laser devices were built, having very little difference in their basic
design. Figure 5-1 shows the basic structure of all of the devices.
The plasma generation section is 91 cm long and consists of a 12-mm
235
O.D. Vycor tube coated on the inside with U 0 by the techniques
O O
described in Chapter 3. The cavity is basically a hemispherical con¬
figuration, consisting of an optical flat mirror 100 per cent reflec-
O
tive from 4500 to 6500 A and a spherical mirror with a 200-cm radius
O
of curvature and 95 to 99.5 per cent reflective from 4500 to 6500 A.
The cavity length of the first device was 199.5 cm, just inside the
stability length of the cavity. This length was used in order to
obtain the largest possible volume in the optical cavity. The second
device (a modification of the first) had a cavity length of 110 cm
and was much easier to align and much more stable. The cavity shape,
design, and spot sizes at critical distances are detailed in Figure
5-3. The rigid aluminum outer shell is the optical bench for the
mirror mounts and the entire structure was placed inside the 9-foot
gas chamber. Cavity alignment was performed with a helium-neon laser.
Gas pressure fills of between 100 and 200 torr were used.
Since the Northrop experimentors [8] indicated problems with
vertical placement of mirrors, such as contamination of the surfaces
with oil and other debris, the laser was first inserted into the hori¬
zontal thermal column of the UFTR (Figure 3-4). At 100 kW reactor
power, the thermal neutron flux available in this region does not
exceed 10 n/cm -sec.

Figure 5-1
Nuclear Pumped Laser

182
At 100 kW a red glow was seen at the exit mirror of the laser.
This was a viewing distance of 7 feet. The blue component of the
plasma was blocked by the 97 per cent reflectivity of the mirror in
the blue region. No indication of lasing was seen.
Since the available thermal neutron flux in the thermal column
was low over the length of the foil section, the second device (a modi¬
fication of the cavity length of the first device from 199 cm to 110 cm)
was placed in the center vertical port where flux levels of 3 x 10’*’*
2
n/cm -sec were measured. The results at this location were very
encouraging.
There are two possible conclusions that could be drawn from
these results: the laser was either lasing or not lasing. The follow¬
ing evidence is presented:
1. A light spot was observable by the eye, only when the
eye was positioned in one exact location.
2. The spot was very bright compared to the hazy blue back¬
ground. This is quite different than the dim red output
observed when the laser was in the thermal column.
3. A phenomenon called "laser speckle," which is seen by the
eye and is associated with all visible laser light, was
definitely in evidence. This effect is due to the inter¬
ference fringes around a coherent beam of light.
4. The observable spot was in the blue-green region where the
laser output mirror is 97 per cent reflective.

183
5. The photographs in Figure 5-2 indicate that there was
definitely a spot or collimated beam at the 16-foot loca¬
tion. These plates were taken without any lenses or
filters between the laser and the film surface. Plate A
shows the output at the 7-foot location without the out¬
put mirror mounted on the cavity. Plate B shows the out¬
put at the same location with the output mirror in place.
Plate C is a photograph of the output at the 16-foot posi¬
tion. Note the small spot (circled) with a diameter of
2.5 mm. Plate D was produced at the 16-foot position from
a mockup of the laser experiment. A tungsten filament
lamp and diffuser replaced the bottom mirror and the top
mirror was removed.
The output from the device was decreasing rapidly when Plate C
was taken, and a later photograph showed nothing. The spot on Plate C
was located in the same position that an observer's eye had to be in
order to see the blue-green spot.
If one assumes the device was not lasing, the following items
would result:
1. Laser speckle would not be present.
2. The beam at the 16-foot distance would be collimated by the
chamber wall dimensions to a spot about 4 in. in diameter
(see Figure 5-2, Plate D).
The evidence thus tends to negate the proposal that the device
was not lasing. Absolute proof of lasing can only be made by measuring

Figure 5-2 Nuclear Pumped Laser Output
184

185
the output for coherence with an interferometer. The output faded so
quickly that neither this nor spectroscopic measurements were made;
neither coherence nor single wave length output can be proved.
If lasing is assumed, the spot size at 16 feet (Figure 5-3)
would be approximately 3.24 mm. The spot size on Plate C of Fig¬
ure 5-2 is similar in diameter (2.5 mm). Due to the low output of the
system the edge of the measured spot may not have been recorded on
the film.
Upon removal from th>e reactor and disassembly of the chamber,
the pungent odor from the chamber indicated the breakdown of the small
amount of silicone sealer that was used to fix mirror alignment. The
output mirror coating had been destroyed, probably by the chemical
effects of the silicone sealer products. This explains the loss of
photon output.
Encouraged by the results of the second laser, the author
designed and built a third device with much improved optical mounts.
The pumping and filling apparatus was changed to a system allowing
“6
pump down to 10 torr and fill with ultra-pure gas. The optical cavity
was similar except for new mirrors of higher quality.
Results from this experiment were similar; however, a photo¬
graph of the spot could not be obtained at the 16-foot distance. This
was perhaps due to a misalignment of the film with respect to the
4-inch cylindrical tube used to shield the film from extraneous light.
This is suspected because the viewing location for the spot was at the
edge of the cylindrical tube.

mirror mirror
= 4380 A
w.
w.
wr
1
gd-g)
1
4
Figure 5-3 Cavity Design

187
The output was slightly higher, due most likely to the decrease
in charge transfer reactions (equation (36)) with nitrogen and water
impurities. Further work, such as gain measurements, is presently
being completed on this device.
In conclusion, if lasing did occur in this experimental device,
an increase of several orders of magnitude in thermal neutron flux,
a magnetic constriction of the plasma into the cavity area, and improve¬
ment in the design of the cavity could result in a sizable increase in
output power. Thus, by the use of interferometric and spectroscopic
methods, absolute proof of lasing would be in evidence.
5.2 A Neutron Detector for the Liquid
Metal Fast Breeder Reactor
For the last few years, engineers have been plagued with
problems while using conventional detectors for monitoring neutron
flux in fast breeder reactors. These difficulties are due to the
rather severe environment seen by all internal reactor neutron detectors.
Not only must these detectors be very small (1/4 inch diameter)
in order to fit in the compact core, they must be able to withstand
9
a 2000°F temperature along with a gamma dose rate of 10 R/hr.
Thermal shocks are expected to be extreme, for example, a 100°F change
in three seconds or a 600°F change in one minute. Throxigh all this,
the detectors must last at least one year and monitor a fast neutron
flux over at least two orders of magnitude. Presently available
devices cannot withstand this environment; therefore, plans for LMFBR's
include either continuous replacement of in core detectors or external

188
to the core placement of compensated ion chambers. Both of these
methods are not adequate and cannot be the ultimate solution.
The fission fragment-generated plasma detector offers an
excellent alternative to the present devices. As will be seen, it does
not include hardware that will degrade in the LMFBR.
Examination of the failure modes of the conventional detectors
(fission chambers, compensated ion chambers, thermocouples, self-
powered devices) shows that the biggest problem is transmission of
data from the detector. There is considerable degradation of the low
output signal largely due to increased leakage currents and noise in¬
duced into the insulators and cables leading to the sensors. This
degradation is due mainly to high temperature and high gamma doses
9
(10 R/sec). Also, a detector with good discrimination against this
extremely high gamma background is a necessity.
These problems are, as described, not applicable to the
plasma detector. Information is transmitted by photon energy to an
external detector and the foils and container are not affected by the
high temperatures or thermal shocks.
The plasma detector in preliminary form is shown in Figure 3-1.
It is identical to the fission fragment interaction device except for
external diagnostic and power systems. Operation of this detector is
based upon the following premise:
The number density of fission fragments being generated
by the foil is a linear function of the number of fissions and,
thus, the neutron flux arriving at the foil. If it is assumed
that the intensity of the optical output generated in argon

189
by the fission fragments is a linear function of the fission
source, then the photon intensity is a linear function of the
neutron flux.
If this can be proved valid, the detector is an excellent
neutron flux monitor. But, the system does present several diffi¬
culties not present in conventional devices:
1. The photomultiplier photon detector is extremely sensitive
to gamma background, thus providing a DC shift on the out¬
put that is a function of the gamma environment of the
reactor.
2. The gas is subjected to gamma interactions; thus,
Compton, pair production, and photoionization processes
will occur, giving rise to false output.
3. Optical systems cannot survive the reactor environment
without darkening of the windows and lenses and damaging
mirrors (if present).
Fortunately, these problems can be overcome. First, in order
to eliminate all extraneous effects in the photomultiplier detector,
the light intensity of the "plasma” is modified by field amplification,
using a periodic pulse input. The output of the photomultiplier is
then filtered and the resultant signal is a direct measure of neutron
flux.
The second problem can be minimized by both calibration and
detection methods involving discrimination against certain wave
lengths. For instance, at the low pressures used in this detector,

190
the predominant energy transfer mechanism for gamma generated excita¬
tion (Compton scattering) produces excited species (AR I) and un¬
ionized species (Ar II). Therefore, the argon II states will be
predominantly generated by heavy particle interactions. As noted in
Chapter 4, the argon II lines are located in the blue region and the
argon I lines in the red region. Simple optical filtering of red
and U.V. region light would allow output from the argon II lines only.
The third problem, survival of an optical system, can be
bypassed. Since light can easily be transmitted by reflection up the
polished interior of a chamber and even around a 90° arc without the
use of any mirrors or lenses, all optical devices can be removed from
primary exposure. The exit window of the chamber can then be located
in a position of low gamma and neutron levels.
Energy losses, other than spontaneous emissions such as charge
transfer to impurity atoms and molecules, should be investigated in
the future as a possible degradation effect on the photon emission.
5.2.1 Diagnostic and Power Supply Systems
Although future output measuring equipment may include
digital filtering and readout, the initial diagnostic equipment used
to verify the operation of this detector consists of elementary analog
devices. This equipment was assembled in the order shown in Figure 5-4.
Field modulation is supplied by a 600-volt square wave generator signal
placed on the electrodes of the fission fragment chamber (Figure 3-3).
Initial tests using a sinusoidal modulation signal were not successful
for an unexplained reason. The square wave generator provides ample

Figure 5-4 LMFBR Neutron Detector Signal Flow
191

192
modulation of the photon output. Also, the output voltage was not
altered by variations in frequency from 0 to 100 Hz (the range of the
square wave generator). The photon output was passed up the chamber
and reflected 90° to a filtering system or spectrograph located exter¬
nal to the reactor. It should be noted again that the lens shown in
Figure 3-1 does not have to be present.
From the optical filtering system, light is passed to a photo¬
multiplier whose electrical output signal is processed through a band
pass filter. The signal is then displayed on an oscilloscope along
with the input signal to the chamber electrodes. The voltage of the
sinusoidal output signal should be a function of the neutron flux
impinging on the uranium coatings.
5.2.2 Neutron Detector Experimental Results
All measurements are referenced to a standard compensated ion
chamber located in the reactor. Of the three gases investigated,
argon gave the most encouraging results. CF^ gave no measurable field
amplification and is also not suitable due to the effects described in
Chapter 4. Helium has a sparce, spread out spectrum, thus providing
difficulties in obtaining large photon output variations of its lines.
Also, helium is notoriously sensitive to charge transfer mechanisms
and the formation of molecular helium ions, thus decreasing the photon
output.
Argon has a profuse line output with the predominant grouping
of Ar I lines in the red region and Ar II lines in the blue region.
Both sets of lines are easily separable by filtering techniques and
both have large photon outputs.

193
Figure 5-5 shows the excellent linearity of the line output
given by the chamber for a field excitation peak of 20 V/cm. The
O
argon I 6965 A line shows an amplification twice as high as that of
o
the Ar II 4283 A line. This result is similar to the DC data pre¬
sented in Chapter 4. The main purpose of field modulation is to elim¬
inate the effects of gamma in both the photomultiplier detector and
the chamber. Since the predominant effect of photointeractions and
deposition of energy will be excitation of the lower excited states,
it is advantageous to monitor only the argon II lines when in regions
of high gamma radiation. This would increase the discrimination
against gamma deposition and allow more accurate determinations of
nuclear flux. To increase sensitivity of the detector at low reactor
power, usually a region of lower gamma rates, the filtration could be
removed and the total spectrum viewed by the detector. Also, the
switching of optical input would decrease the scaling effort that
would otherwise be needed in order not to saturate the photomultiplier.
The typical output from the detector system as displayed on an
o
oscilloscope is shown in Figure 5-6 for argon I 6965 A. The data
derived from observing one line generated in a flux of 3.8 x 10^
2
n/cm -sec are not encouraging. When the spectrograph was set on the
zero-order point (all light transmitted), the results, as shown in
Figure 5-7, are excellent. Measurable output was obtained for thermal
7 2
neutron flux levels as low as 3.8 x 10 n/cm -sec (10 watts reactor
11 2
power). At 3.8 x 10 n/cm -sec (100 kW) the measured output was
1.3 volts peak to peak. A log-log plot of the data, Figure 5-8, indi¬
cates a linear response down to 500 watts reactor power. The change

LU
CD
z:
rn
o
REACTOR POWER (watts)
Figure 5-5 Amplification of Argon Line Intensity
versus Reactor Power
194

195
INPUT
OUTPUT
INPUT
OUTPUT
1OOy SLITS
lOOy SLITS
Figure 5-6
Ar I 6965 A Filtered Output
Neutron Detector

196
10W 3.8xl0^n/cm2-sec O.OlV/cm
50W
1.9xl0^n/cm2-sec
0.01V/cm
1KW
3.8xl0^n/cm2-sec
0.02V/cm
100W 3.8xl0^n/cm^-sec O.OlV/cm
5KW 1.9xl0^n/cm2-sec 0.05V/cm
100KW 3.8x10 n/cm2-sec 0.5V/cm
500W 1.9xl0^n/cm2-sec O.OlV/cin
80KW 3.04xl011n/cm2-sec 0.5V/cm
Figure 5-7 Total Spectrum Signal - Neutron Detector

VOLTS OUTPUT p-p
REACTOR POWER (Kw)
Figure 5-8 P-P Voltage versus Reactor Power - Neutron Detector
lOOKw
197

198
of slope of the curve indicates an additive constant voltage which is
from a square wave noise signal capacitively coupled from the signal
cables. With the use of proper shielding and separation of the
electronics systems, the output signal would remain a linear function
of neutron flux.
Not only is the response time of this system very short, but
another time-dependent effect was noted. When the reactor was on a
positive or negative period, the output voltage did not follow the
neutron flux. It decreased to a low voltage indicative of the rate
of change of the flux. This unusual effect should be studied for pos¬
sible use as a reactor period indicator. An explanation cannot be
found for this effect at the present time.
5.2.3 Data Projections and
Realistic Chamber Design
There is nothing to indicate that the linearity of the
chamber output would be disturbed at higher flux levels. The peak to
peak output voltage can be presented by the following equation:
V = K $ + B (97)
pp F F
where
2
i = neutron flux n/cm -sec
-11 2
K = 0.3246 X 10 V-cm -sec/neutron
F
B = 0.01667 volts.
F
The constants stated are valid only for this particular experi¬
mental apparatus. If, instead of thermal neutron flux dependence,

199
only fast flux and fission were assumed in this chamber the K value
would be the same, but the V would decrease as the ratio of the fast
PP
-4
to thermal fission cross section, 6 x 10 . Thus, B would be equal
F
to -1.2356. Since the minimum measurable voltage in this system is
10
0.004 volt, the minimum fast flux measurable by this system is 10
2 11 2
n/cm -sec. This level is below the lowest flux, 10 n/cm -sec, con¬
sidered in specifications for an LMFBR neutron detector. Data from
Figure 2-4 indicate that this detector irradiated by thermal neutrons
12
and holding a pressure of 600 torr argon will receive 1.45 X10 MeV/sec.
For a detector whose dimensions are similar to an actual LMFBR device,
0.5 cm I.D. and 125 cm length, Figure 2-3 indicates a unit volume
10 3 „ 11
deposition rate of 10 MeV/cm -sec or a total rate of 6.25 x 10
MeV/sec. This rate is only about half of the energy deposition rate
of the experimental chamber, but the output would still be adequate
10
to give data for fast neutron flux irradiations above 2 x 10
n/cm -sec.
A realistic chamber design would have to specify operation
at pressures much below 600 torr in order to maximize the field
amplification and thus increase sensitivity so that only portions of
the optical spectra need be measured. From the data in Chapter 4, it
is evident that a chamber pressure between 50 and 100 torr will give
maximum gain.
The installation of a coaxial electrode structure with porous
U„0 coatings on the interior of the outer electrode will allow much
3 8
greater field strengths than the 20 V/cm maximum for the ring electrode

200
structure. Field amplification and thus the system sensitivity would
again be greatly improved.
235
It must be noted that coatings are not limited to U~
Boron coatings which react to give a high energy alpha particle
are also candidates for this type of chamber. There is also a dis-
3
tinct possibility of using the He (n,p)T reaction without the coatings
to produce a plasma.
Pressure measurements in the chamber can be related to the
temperature seen by the chamber. Thus this device could also indi¬
cate the thermal temperature of the reactor. Since the ideal gas law
is approximately correct for argon ,
T°K = —— , (98)
nR
pressure can supply a value for the mean temperature of the chamber
gas fill. Since energy deposition by the fission fragments is a func¬
tion of the number density of the atoms and not the pressure, the
elevated temperature will not affect the integrated optical output.
This detector system meets all of the basic requirements of
an LMFBR neutron detector. It should be investigated in great detail
in order to establish the most advantageous structure, species,
spectral region, and gas pressure for maximum output and discrimina¬
tion against gamma background.

CHAPTER 6
CONCLUSIONS
The excellent results from the spectroscopic study of in-reactor
plasmas has shown that this type of research is possible and extendable
to many types of devices and gases. The experimental techniques that
are presented herein seem quite adequte for investigations of gases
whose reactions are unaffected by impurity species. For future studies
of gases it is recommended that a high-quality vacuum system be installed
in very close proximity to the experimental chamber so that gas fills
using high purity gas can be utilized. Out-gassing of the chamber can
also be aided by operation of the reactor while the chamber is under
high vacuum. In addition, in future investigations, the ring anode
should be replaced by an axially symmetric device with the porous coat¬
ing placed on the inside of a metal sleeve. This will allow observa¬
tion of the foil surface and eliminate the shadowing effect of a ring
anode.
The coating procedures developed seem to produce an excellent
foil with the techniques applicable to many surfaces and many metal
oxides. The two important advantages of this chemical technique are,
first, a thick large-surface porous coating is produced, unlike the
flat, dense coating produced by vacuum deposition; and, second, these
coatings can be produced without any sophisticated equipment.
201

202
The spectroscopic analysis of helium and argon yielded a large
amount of spectral data with the surprising inclusion of He II and
Ar III as emitting species. The kinetic processes in these gases and
included impurities have been established with analysis giving Boltzmann
temperatures and relative excited state densities. The discovery of
several possible Ar II population inversions has given encouragement
to the further development of the nuclear-pumped argon ion laser.
From probe analysis, the electron densities were found to be
10-3
around 1 x 10 e /cm from gases bombarded by fission fragments from
11 2
the reactor at a thermal neutron flux of 3.8 x 10 n/cm -sec. The
experimental values of ion pair generation rates compared favorably
with the stopping power calculations of Chapter 2. Thus, such
averaged deposition calculational techniques seem capable of predict¬
ing the energy deposition from fission fragments generated in a foil.
The non-Maxwellian electron energy distribution developed from
noncommunicating energy bands has compared favorably with Monte Carlo
calculations, with the presence of a high energy tail on the distribu¬
tion well established.
A photon amplification factor (a) for Ar I and II has been
developed, where ot/p is expressed as a function of E/p. This func¬
tion allows the calculation of the exponential amplification of a line
intensity by application of a field across the plasma. The values for
Ar II were found to approach the Townsend ionization coefficient, as
would be expected.
The above results all show that there is no group model now
available to describe the fission fragment-produced plasma adequately.

203
Therefore, further research into this area should include the develop¬
ment of a rate equation set that adequately characterizes the transi¬
tion involved in the plasma. To this end, the unknown factors are now
the generation coefficients for direct population of the excited states.
Since the branching ratios of the states have for the most part been
described, such generation data are available, utilizing the equipment
of this research. The only modification that would be required would
be the use of ultra-pure gases (and maintenance of the purity at less
than 0.1 ppm), and the absolute calibration of the optical system.
It is felt that until this research is completed (for mixed energy
fission fragments), no model will be valid.
The development of the LMFBR detector system is an excellent
use of the techniques and theory developed herein. Further study of
this device is essential; with improved geometry and optical transmis¬
sion system and a more stable gas, a valuable device for fast neutron
detection will be operative.
The findings showing that a mixed source of radiation acts on
only the cathode of a glow discharge (within the constraints of the
experiment) will generate new schemes for enhancing the output of
a laser. It is evident that gamma radiation of a CO laser cathode
will aid in keeping the thermal temperature low by allowing a lower
power input to maintain the discharge. Thus, the laser efficiency and
power output will increase.
Laser pumping by nuclear sources has been investigated by many
researchers with no results showing positive proof of lasing. The
device described herein has probably approached lasing or has lased at

204
very low output. The spectroscopic analysis of argon has shown that
the argon ion is populated far above the level normally associated with
its Boltzmann temperature. Thus, there is great encouragement that
further research will produce an argon ion laser with easily measurable
output. Better laser design and larger neutron flux inputs can only
aid in this purpose.
The spectroscopic results and laser techniques are especially
applicable to the study of gases that may lead to high-output pure
nuclear-pumped lasers. Such gases could include UF at high pressure
6
and elevated temperatures where bands systems available only by high-
energy particle bombardment (fission frequency), as was found here in
CF , could be made to show lasing action. The substitution of a liquid
4
in place of the gas should present no problems for a similar study.
The liquid medium for lasing has the largest energy transfer, except for
solids; using carrier liquids that show little degradation in the
nuclear-pumped laser may be possible.

APPENDIX I
PRESSURE DEPENDENCE OF RELATIVE LINE INTENSITIES
AND EXCITED STATE DENSITIES - HELIUM

RELATIVE INTENSITY
206
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ HELIUM HE I 5015*7
x HE I 4321*9

RELATIVE INTENSITY
207
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ HELIUM HE I 7281*3
x HE I 7065-2
4

RELATIVE INTENSITY
208
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ HELIUM HE I 39S4.7
x HE I 3888*6
*b
4

RELATIVE INTENSITY
209
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ HELIUM HEII 4SS5-7
x HEII 3203*1
Id

RELATIVE INTENSITY
210
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ HELIUM N2+ 4709*2
x N2+ 4G51.8

RELATIVE INTENSITY
211
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ HELIUM N2+ 423S.5
x N2+ 41S6*B
PRESSURE - TDRR

RELATIVE INTENSITY
212
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SPECIES
LINE
+
HELIUM
N3+
3914.4
X
N3+
3357.9
>
N3+
3538-3
<
N3+
3398-7
•to
â– H
100
—i—
£00
I 4 1 1
300 400 500 GOO
PRESSURE - TDRR
700 BOO
4
0

RELATIVE INTENSITY
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SPECIES
LINE
+
HELIUM
NS
4059.4
X
NS
3993.4
>
NS
3755.0
<
NS
3304.9
rl

RELATIVE INTENSITY
214
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SPECIES
LINE
+
HELIUM
N2
3671-9
X
N2
357G-9
>
N2
3371-3
<
N2
3153-3
•to
100
-i
200
300 400
PRESSURE
' 500 GOO
- TDRR
700
"boo
4
o

RELATIVE INTENSITY
215
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ HELIUM HP 65SP•7
x HP 4861*3
*b
t

RELATIVE INTENSITY
216
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SFECIES LINE
+ HELIUM CC2+ 28SS-0
x C02+ 2083-0
*b

RELATIVE INTENSITY
217
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ HELIUM CO0 3839-8
x C02 3084-0
Id
*¡b
•to
—i
200
—i
400
100
300
500
600
700
BOO
PRESSURE - TÃœRR
o

RELATIVE INTENSITY
218
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SFECIES LINE
+ HELIUM 02+ 3733.9
x 02+ 3621*0

RELATIVE INTENSITY
219
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ HELIUM CN 4515-0
x CN 3585•S

LDG(LAMBDA*I/G*A)
220
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
5 > O-
4.Q-
2-0-
l.Q-
0*0
POINT
GAS
SPECIES
LINE
EU
+
HELIUM
HE I
7281*3
22*92
X
HE I
70S5-2
22*72
t>
HE I
GS78-1
23*07
«
HE I
5875*G
23*07
—•*-
—t—
100
—i—
EDO
300 400 500
PRESSURE - TGRR
BOO
700
BOO

LDG(LAMBDA"I/G"A)
221
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SPECIES
LINE
EU
+
HELIUM
HE I
5015-7
23-09
X
HE I
4321*9
23-74
HE I
4471-5
23-73
4
HE I
4307 *3
24*04
4*0-
—i—
300
—f—
400
—t-
000
soo
GOO
700
PRESSURE - TDRR
o-o
o
H
100
—
200

LOG(LAMEDA»I/G*A)
222
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE EU
+ HELIUM HE I 33S4-7 23-74
x HE I 3B8B• G 23-01

APPENDIX II
BOLTZMANN TEMPERATURE PLOTS
HELIUM

LOG(LAMBDA-I/G-A)
224
BOLTZMANN PLOT
SPECIES-HELIUM I
PRES— 25 TDRR
BDLTZ• TEMP— 4553-1 DEG- K

LOG (LAMBOA"I/G*A)
225
BOLTZMANN PLOT
SPECIES-HELIUM I
PRES— 50 TORR
BOLTZ• TEMP•= 3374-2 DEG- K
4-0
3-0
2*0
1-0
!
0*0.
22
-H ^ ♦ ♦ + 1 c?4
UPPER STATE ENERGY - EV
+
+

LOG(LAMBDA»I/G"A)
226
BOLTZMANN PLOT
SPECIES-HELIUM I
PRES•= 100 TDRR
BDLTZ• TEMP» = 4160-2 DEG* K
4

LOG(LAMBDA"I/G"A)
227
BOLTZMANN PLOT
SPECIES-HELIUM I
PRESâ– = BOO TDRR
BDLTZ» TEMP»- 355B-1 DEG* K
4.0
3«0 •
2-0
1*0-
O.Q
t
H 1 1 h-
H h-
~^A ' f
22
UPPER STATE ENERGY - EV

LOG(LAMBDA-I/G*A)
228
BOLTZMANN PLOT
SPECIES-HELIUM I
PRES•= 400 TDRR
BDLTZ• TEMP * = 3442-3 DEG- K

229
BOLTZMANN PLOT
SPECIES-HELIUM I
PRES * = 760 TDRR
BDLTZ• TEMP•= 3716-4 DEG- K
«

LOG (LAMBDA**I/G**A)
BOLTZMANN PLOT
SPECIES-HELIUM I
PRES-= 5»7 TCRR
GLOW DISCHARGE
BDLTZ• TEMP— 5020-2 DEG- K

APPENDIX III
PRESSURE DEPENDENCE OF RELATIVE LINE INTENSITIES
AND EXCITED STATE DENSITIES - ARGON

RELATIVE INTENSITY
232
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SFECIES
LINE
+
ARGON
AR I
B103
X
AR I
7G35
AR I
BOOS
AR I
7514
'lb
‘Tb
100
—i—
200
3X> 400
PRESSURE
500 GOO
- TQRR
700
BOO
<
0

RELATIVE INTENSITY
233
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON AR I 8115-3
x AR I 8014-8

RELATIVE INTENSITY
234
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON AR I 7948-2
x AR I 7724-2
4

RELATIVE INTENSITY
235
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON AR I 7304.0
x AR I 7272*9
4

RELATIVE INTENSITY
236
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON ARII 4348.1
x ARII 426S•5
w |p|

RELATIVE INTENSITY
237
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON ARII 4475-0
x ARII 4440-0

RELATIVE INTENSITY
238
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON ARII 4726•S
x ARII 4657 *3
4

RELATIVE INTENSITY
239
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON ARII 3S94.8
x ARII 4583*9

RELATIVE INTENSITY
240
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON ARII 3431-5
x ARII 37BO.0

RELATIVE INTENSITY
241
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SFECIES LINE
+ ARGON ARII 3729*3
x ARII 3050.G
IK a.11

RELATIVE INTENSITY
242
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON ARII 4103-9
x ARII 3770.5

RELATIVE INTENSITY
243
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON ARII 4373-7
x ARII 4073*3

RELATIVE INTENSITY
244
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON ARII 4052-3
x ARII 4449.3
^ ARII 3724.5
4

RELATIVE INTENSITY
245
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON ARII 3293-G
x ARII 3744.3
4

RELATIVE INTENSITY
246
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON ARII 3520•0
x ARII 3582*4
4

RELATIVE INTENSITY
247
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON ARII 4277-5
x ARII 4131-7

RELATIVE INTENSITY
248
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON ARII 4401- 0
x ARII 4906-0

RELATIVE INTENSITY
249
*b
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON ARIII 3480.G
x ARIII 3391*9
â– to
100
230
300 4(00 S&5 6Ü0
PRESSURE - TDRR
7^0 BOO
4
0

RELATIVE INTENSITY
250
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SPECIES
LINE
+
ARGON
OH
3472*0
X
OH
3009.0
>
OH
3070-0
<
OH
3007.0
*b
‘to
3X1
<00
500
600
PRESSURE - TGRR
BOO
100
loó
-)—
700

RELATIVE INTENSITY
251
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
FDINT GAS SPECIES LINE
+ ARGON OH 2829•0
PRESSURE - TDRR
«

RELATIVE INTENSITY
252
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SFECIES LINE
+ ARGON NS 3371-0
x N2 31EQ-1
4
X) fz-»o+

RELATIVE INTENSITY
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON N2 3116«7
x N2 2976.B

RELATIVE INTENSITY
254
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SPECIES
LINE
+
ARGON
N2
3642-0
X
N2
3577-0
>
N2
3537.0
<
N2
3463-0
°o
I
•to
100
200
abo áoo seo gbó
PRESSURE - TDRR
7 00
BOO
4
0

RELATIVE INTENSITY
255
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
♦ ARGON N2 4263*0
x N2 4053*0
4

RELATIVE INTENSITY
256
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SFECIES LINE
+ ARGON N2+ 3804.0
-b
4

RELATIVE INTENSITY
257
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SPECIES
LINE
+
ARGON
COS
35SS-0
X
COS
3546-0
COS
3510-8
4

RELATIVE INTENSITY
258
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGON CO 3680*9
*b

RELATIVE INTENSITY
259
SPECTRAL INTENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE
+ ARGGN CO+ 3525*0
•b
4

LGG(LAMBGA*I/G*A)
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SPECIES
LINE
EU
+
ARGON
AR I
8115.3
13*08
X
AR I
8014-8
13-03
>
AR I
8284.5
13-33
AR I
7723-8
13-15
2*0”
1*0-
0-0
1C»
200
300
400
500
GOO
700
PRESSURE - TDRR

LOG (LAMBDA** I/G»A)
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SPECIES
LINE
EU
+
ARGON
AR I
4130-7
14-51
X
AR I
4161•3
14-63
AR I
3343-0
14-63
<
AR I
4653*4
14.74
2-0-
1*0
0-0
+
1C»
—t—
200
—I 1—
300 400
PRESSURE -
■H—
500
TDRR
0
-H
E00
—I—
700
000

LOG(LAMBDA-I/G»A)
262
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT GAS
+ ARGON
SPECIES
AR I
AR I
LINE
7348*2
7724*2
EU
13*28
13*33

LOG(LAMBDA*I/G*A)
263
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SPECIES
LINE
EU
+
ARGON
AR I
7304-0
13-30
X
AR I
7272-3
13-33
AR I
G3G5•4
13-33
<
AR I
4200-7
14-50
3.0-
2.0"
1*0
0-0-1 > 11 1 1 1 t ^
0 100 £00 300 400 500 GOO 700 BOO
PRESSURE - TORR
4

LOG(LAMBDA-I/G-A)
264
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SPECIES
LINE
EU
+
ARGON
AR I
0103.7
13-15
X
AR I
7G35.1
13-17
AR I
0COG•2
13-17
<
AR I
7514*7
13-27
2*0
1*0
0.0
■H 1—
300 400
PRESSURE -
—i—
500
TURR
-i *-
700 BOO
4
0
-I—
100
—I—
£00
—I—
BOO

LOG(LAMBDA*I/G*A)
265
5-Of
4.0-
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE Ell
+ ARGON ARII
x ARII
t> ARII
4052-3 23*BO
4443.3 24-20
3724-5 24.02
3-0-
0-0
-+
BOO

LOG (LAMBGA**I/G*A)
266
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SPECIES
LINE
EU
+
ARGON
ARII
4035-5
21-50
X
ARII
4072-0
21-50
>
ARII
4481-B
21-50
<
ARII
4301-0
21-50
4.Q-
3-0-
0-0-1 1 1 1 1 1 1 • *■
0 100 200 300 400 500 EOO 700 BOO
PRESSURE - TGRR
4
+*+

LOG(LAMBGA**I/G*A)
267
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SPECIES
LINE
EU
+
ARGON
ARII
4401-0
13-22
X
ARII
4806*0
13*22
ARII
4371*3
13-26
<
ARII
4013*3
13-43
4-0
3*0
2-0 •
300 400 SCO BOO
pressure: - TCRR
700
BOO
o-o
0
—t—
100
—I—
200

LOG(LAMBGA*I/G*A)
268
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SFECIES LINE EU
+ ARGON ARII 3491*5 92*77
x ARII 3780*8 92*77

LOG(LAMBDA"I/G-A)
269
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SFECIES
LINE
EU
+
ARGON
ARII
4103-9
22-51
X
ARII
3770-5
22-59
>
ARII
4156.1
22-59
<
ARII
4103-8
22-70
4.0
3.0
2-0
1*0
4

LOGCLAMBDAhI/G-A)
270
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE EU
+ ARGON ARII 4348-1 19-43
x ARII 4SS6.5 19-55
PRESSURE - TORR

LOG(LAMBDA*I/G-A)
271
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE EU
+ ARGON ARII 3723•3 13*37
x ARII 3S50.G 13*37

LOG(LAMBOA-I/G-A)
272
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT
GAS
SFECIES
LINE
EU
+
ARGON
ARII
3520•0
23-07
X
ARII
35S2•4
23-07
ARII
3373-4
23-00
<
ARII
38SB «5
23*17
4.Q-
3.0"
2.0
0*0
—t-
800

LOG(LAMBDA»I/G*A)
273
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SFECIES LINE EU
+ ARGON ARII 4277.5 21-35
x ARII 4131*7 21-43

LOG (LAMBDA **I/G** A)
274
POPULATION DENSITY
GAS TEST GE1_L EXPERIMENT
POINT GAS SPECIES LINE EU
+ ARGON ARII 3934.8 80*74
x ARII 4589-9 81-13

LOG(LAMBDA*I/G»A)
POPULATION DENSITY
GAS TEST CELL EXPERIMENT
POINT GAS SPECIES LINE EU
+ ARGON ARII 4725.9 19-75
x ARII 4S57.5 19*80

LOG(LAMBDA"I/G"A)
276
POPULATION DENSITY
GAG TEST CELL EXPERIMENT
POINT
GAS
SPECIES
LINE
EU
+
ARGON
ARII
4373*7
13*54
X
ARII
4873*3
13*58
>
ARII
4288*2
13*58
ARII
4355*1
13*75
4*0-
3 • 0
2*0-
o • 0-1 i i < 1 1 1 1 f
0 100 KOO 300 400 500 600 700 DOO
PRESSURE - TORR
4

APPENDIX IV
BOLTZMANN TEMPERATURE PLOTS - ARGON

LOG(LAMBDA*I/G*A)
278
BOLTZMANN PLOT
SPECIES - ARGON I
PRES•= 25 TDRR
BOLTZ» TEMP• = **»*»»* DEG• K

LOG(LAMBDA-I/G-A)
279
BOLTZMANN PLOT
SPECIES - ARGON I
PRES -= 75 TORR
EDLTZ• TEMP» = 37301-3 DEG- K

LOG (LAMBDA*I/G*A)
280
BOLTZMANN PLOT
SPECIES - ARGON I
PRES•= 150 TDRR
BOLTZ- TEMP— E0631-7 DEG- K
4

LOG(LAMBDA*I/G*A)
281
BOLTZMANN PLOT
SPECIES - ARGON I
PRES•= 204 TDRR
BOLTZ- TEMP *= 24301-6 DEG- K

LOG(LAMBDA-I/G-A)
282
BOLTZMANN PLOT
SPECIES - ARGON I
PRES•= 450 TDRR
BGLTZ• TEMP•= 15840-0 DEG- K
4

LOG (LAMBDA *♦ I / G ** A)
283
BOLTZMANN PLOT
SPECIES - ARGON I
PRES•= BOO TDRR
BDLTZ• TEMP-= 1405B-5 DEG- K
4

LOG(LAMBDA-I/G"A)
284
BOLTZMANN PLOT
SPECIES - ARGON I
PRES— 760 TORR
BOLTZ• TEMP— 17321-5 DEG- K
4

285
BOLTZMANN PLOT
SPECIES - ARGON II
PRESâ– = 25 TORR
BOLTZ- TEMP•= 55454-6 DEG- K

BOLTZMANN PLOT
SPECIES - ARGON II
PRES•= 75 TDRR
BDLTZ- TEMP»- SBEB0»0 GEG» K

LOG(LAMBDAHI/GHA)
287
BOLTZMANN PLOT
SPECIES - ARGON II
PRES•= 150 TORR
BOLTZ• TEMP-= 77508-3 DEG- K
4

288
BOLTZMANN PLOT
SPECIES - ARGDN II
PRES *= 2B4 TDRR
BDLTZ• TEMP• = 33804-0 DEG* K

289
BOLTZMANN PLOT
SPECIES - ARGON II
PRES-- 450 TORR
BOLTZ- TEMP»= BEEBE-7 DEG- ft
¿5

BOLTZMANN PLOT
SPECIES - ARGON II
PRES— GOO TDRR
BOLTZ- TEMP— 60430-3 DEG- K

291
BOLTZMANN PLOT
SPECIES - ARGON II
PRES•= 760 TORR
EOLTZ» TEMP— G2617-3 DEG- K

BOLTZMANN PLOT
SPECIES - ARGON II
PRES -= BOO TORR
EO V/CM ELECTRIC FIELD
BOLTZ■ TEMP•= ******* DEG• K

LOG(LAMBDA-I/G"A)
BOLTZMANN PLOT
SPECIES - ARGON I
PRES— 4*7 TORR
GLOW DISCHARGE
BDLTZ» TEMP— ******* DEG- K

BOLTZMANN PLOT
SPECIES - ARGON II
PRES — 4.7 TGRR
GLOW DISCHARGE
BDLTZ- TEMP— 35765-6 DEG- K

APPENDIX V
FIELD AMPLIFICATION OF ARGON SPECTRAL EMISSION

CURRENT (amps) xlO
296
0 100 200 300
VOLTAGE
Amplification and Current Versis Applied Voltage -
25 torr Argon with 30.5 cm Electrode Seperation
AMPLIFICATION

CURRENT (arnps) xIO
297
200 300 400 500
VOLTAGE
Amplification and Current versis Applied Voltage -
75 torr Argon with 30.5 cm Electrode Seperation
AMPLIFICATION

CURRENT (amps) xlO
298
200 400 600
VOLTAGE
Amplification and Current versis Applied Voltage -
150 torr Argon with 30.5 cm Electrode Seperation
AMPLIFICATION

CURRENT (amps) xlO
299
VOLTAGE
Amplification and Current versis Applied Voltage -
284 torr Argon with 30.5 cm Electrode Seperation
AMPLIFICATION

CURRENT (amps) xIO
300
Amplification and Current versis Applied Voltage -
450 torr Argon with 30.5 cm Electrode Seperation
AMPLIFICATION

CURRENT (amps) xlO
301
Amplification and Current versis Applied Voltage -
760 tott Argon with 30.5 cm Electrode Seperation
AMPLIFICATION

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BIOGRAPHICAL SKETCH
Roy Alan Walters was born October 19, 1941, in Rockville Centre,
New York. Upon graduation from Wantagh High School he attended the
University of Florida, from which he received the Bachelor of Electrical
Engineering degree in December of 1964. In June of 1966, he obtained
his Master of Science in Nuclear Engineering from the Georgia Insti¬
tute of Technology, Atlanta, Georgia, specializing in reactor engineer¬
ing and radiological health physics.
Mr. Walters will always look back with special affection on
the past two years which he spent as caretaker of the "Gator Ski Club
and Sail Club" property on Lake Wauburg. To have been able to live in
the midst of the abundance of nature's peace and beauty was a rare
privilege which softened the sharp edges and brought new perspectives
to an often too scientific existence.
Mr. Walters, his wife, Linda, and their son, Jason, presently
reside in Orlando, Florida, where he is employed by Martin Marietta
Corporation.
308

I certify that I have read this study and that in my opinion it
conforms to acceptable standards of scholarly presentation and is fully
adequate, in scope and quality, as a dissertation for the degree of
Doctor of Philosophy.
Richard T. Schneider, Chairman
Professor of Nuclear Engineering Sciences
I certify that I have read this study and that in my opinion it
conforms to acceptable standards of scholarly presentation and is fully
adequate, in scope and quality, as a dissertation for the degree of
Doctor of Philosophy.
/ William H. Ellis
Associate Professor
of Nuclear Engineering Sciences
I certify that I have read this study and that in my opinion it
conforms to acceptable standards of scholarly presentation and is fully
adequate, in scope and quality, as a dissertation for the degree of
Doctor of Philosophy.
George R. Dalton
Professor of Nuclear Engineering Sciences
I certify that I have read this study and that in my opinion it
conforms to acceptable standards of scholarly presentation and is fully
adequate, in scope and quality, as a dissertation for the degree of
Doctor of Philosophy.
of Nuclear Engineering Sciences

I certify that I have read this study and that in my opinion it
conforms to acceptable standards of scholarly presentation and is fully
adequate, in scope and quality, as a dissertation for the degree of
Doctor of Philosophy.
Kwan Chen
Associate Pro^ssor
of Physics and Astronomy
I certify that I have read this study and that in my opinion it
conforms to acceptable standards of scholarly presentation and is fully
adequate, in scope and quality, as a dissertation for the degree of
Doctor of Philosophy.
Miku*atf'3. Ohanian
Professor of Nuclear Engineering Sciences
This dissertation was submitted to the Dean of the College of Engineering
and to the Graduate Council, and was accepted as partial fulfillment of
the requirements for the degree of Doctor of Philosophy.
June, 1973
Dean, Graduate School

UNIVERSITY OF FLORIDA
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