NUCLEAR INSTRUMENTS AND METHODS 67 (I969) 343-347;
T H E R E S T R I C T E D ENERGY LOSS CRITERION
F O R REGISTRATION OF CHARGED PARTICLES IN PLASTICS*
E. V. BENTON and W. D. NIX t
U. S. Naval Radiological Defense Laboratory, San Francisco, California 94135, U. S. A.
Received 26 July 1968
It was found that the restricted energy loss rate of charged
particles can be used as a convenient criterion to predict the
formation or non-formation of etchable tracks in plastics. The
criterion allows sensitivity assignments, in absolute units, to
each of the polymeric detectors. An experimentally determined
parameter indicates that only electron energy transfer collisions
of about 1.0 keV and less are important in track formation.
1. Introduction
Plastics are currently being used as detectors for
heavily ionizing charged particles for certain studies in
nuclear physics, astrophysics, and geophysics1). In these
detectors, paths of individual charged particles are
revealed by a selective chemical etching of the radiation
damaged material along the particle trajectory. Their
principal usefulness lies in the ability to register only
particles possessing ionization above some threshold
value.
The ability to predict which particles will produce
latent (etchable) tracks in a given polymer is a basic
requirement to understanding of the chemical etch
phenomenon. It is also essential to the practical utili-
zation of the detectors. Previously two track registra-
tion criteria were proposed; one based on the total
rate of energy loss (dE/dx)crit2), and the other on the
rate of primary ionization (PI) of the bombarding
particle3). Subsequent experiments showed that the
(dE/dx)crit criterion failed at high velocities of the
bombarding particle3-5). The PI criterion while in
agreement with the known experimental data, never-
theless has some difficulties associated with it6). The PI
criterion makes use of an expression of Bethe 7) [eq. (1),
p. 45 Of 7)] t o calculate the rate of primary ionization.
Since the dimensionless constants r and s, which appear
in this expression, have been calculated for only one
stopping material (hydrogen), the absolute values of
the primary ionization in plastics are not known.
Relative values must be used in order to calibrate the
plastic detectors3). The Bethe expression also contains
* Segments of this work were sponsored by the National Aero-
nautics and Space Administration, Ames Research Center
(A-65315) and the Manned Spacecraft Center, Houston
(T-68092-G).
t Department of Materials Science, Stanford University.
343
© NORTH-HOLLAND PUBLISHING CO.
The criterion is consistent with the known experimental obser-
vations of charged particle registration in plastics. It is proposed
that latent (etchable) tracks are formed when the energy density
(dose) in the immediate vicinity of the particle trajectory exceeds
a critical value that is characteristic of the particular detecting
material and the specific etching conditions.
the parameters I 0 - the ionization potential of the outer
shell electrons of the stopping atoms. In order to fit the
experimental data on track registration in cellulose
nitrate and Lexan using the PI model, Io = 2 eV must
be used. This value appears to be too low to fit the
physical meaning given to it by BetheT'S). The energy
of 2 eV may suffice to break a chemical bond (raise the
bonding electron to a higher energy state) but, in
general, does not suffice to ionize the atom. For
ionization in plastics, a higher energy of 9 - 15 eV is
required. The criterion is also somewhat physically
unrealistic in that it assumes that the contribution of
secondary and higher order ionizations can be
neglected.
The purpose of this paper is to present a new track
registration criterion which includes the energy
deposited near the particle trajectory as a result of the
higher orders of ionization. The criterion allows
sensitivity assignment in absolute units to all plastic
detectors. It is consistent with the known experimental
observations of track registration in plastics.
2. The restricted energy loss rate criterion
The parameters which influence etching of tracks
can be separated into three broad categories: 1. The
material parameters (including the chemical compo-
sition, molecular weight, molecular chain orientation);
2. The particle parameters (including charge, z; mass,
M; velocity, v); 3. The etching parameters (including
the chemical composition of the etching solution, the
conditions of etching). The question considered in this
paper is: given a particular track detecting material,
how does track registration depend upon the particle
parameters when etching is carried out in a given
specified manner?
 344 E. V. BENTON
We have found that a quantity called the Restricted
Energy Loss (REL) rate of charged particles can be
used to correctly predict track registration in plastics.
The quantity REL is simply the rate of energy loss of
the bombarding particle due to the distant collisions
with electrons of the stopping material. The distant
collisions are defined as those resulting in the ejection
of electrons of energy, co, less than some predetermined
value coo. To adequately represent REL, the energy coo
must fall in the range such that, for close collisions,
the atomic electrons can be treated as free particles,
while for distant collisions the incident heavy particle
is treated as a point chargeT,9).
The quantity REL can be calculated from the follow-
ing expression:
(dE/dx),o<oo = {2 ten(z*) 2 r~ moc2/fl2} •
• [In (2 mo e 2fl 2~ 2 coo/l.~)-fS
2 2 -2(C/Z)-g], (1)
where
z* = effective charge of the ionizing particle;
fl = v/c, the ratio of the velocity of the particle to
the velocity of light, c;
moe z = 0.511 MeV, the rest energy of electron;
n = density of electrons in the stopping material;
ro = e Z / ( m o c 2 ) , the classical electron radius;
y = (1 - f l / ) ~ ;
Iadj = mean excitation potential of the material;
C / Z = tight binding shell correction;
6 = correction for the density effect.
The effective charge, z*, can be obtained from the
empirical relation of Barkas 9) based upon the data of
Heckman et al.~°), for nuclear emulsions:
z* = z [ 1 - e x p ( - 125 13/z})]. (2)
Although strictly true only for nuclear emulsions, eq.(2)
can be used for other solids, except for very heavy ions
at low incident velocities. Because of the computa-
tional uncertainties in the expression used for the C / Z
terms at low energies ~~), eq. (1) strictly holds only above
about 8 MeV/nucleon; however, we have found it to
give satisfactory results down to 3 MeV/nucleon for
particles as heavy as 4°Ar in the polymeric materials
investigated. For particle energies below 3 MeV/nu-
cleon, REL can be obtained by subtracting the energy
lost through close collisions from the total rate of
energy loss,
(dE/dx)~o<,oo -- (de/dX)T-(dE/dx),o>o,o. (3)
The second term on the right-hand side of eq. (3) is
AND W . D. NIX
given by 7,9)
( d E / d x ) o >,oo = {2=n(z*) r 2 m 0
• [In (co~..JOOo)-32], (4)
where
COmax = {2fl2/(1-[~2)} mo c2 . (5)
In this work coo is treated as an adjustable parameter.
It is the average energy of the recoil electrons that
delineates the boundary between those electrons which
contribute and those that do not contribute to the
formation of latent tracks. It was found that a value
of coo = (1.0+_0.2)× 10 a eV gave the best agreement
with experimental data (for the polycarbonate plastic
this is only an approximate value). In figs. 1 and 2 the
restricted energy loss rate (dE/dx)o< lo~, is plotted as a
function of energy per nucleon for a number of heavy
ions in cellulose nitrate and polycarbonate resin
plastics, respectively. The theoretical curves of figs. 1
and 2 are generated in the following way. In the energy
interval from 0.1 to 0.5MeV/nucleon the total
( d E / d x ) is used since comax --< 103 eV. Above 0.5 MeV/
nucleon the values given by eq. (4) are subtracted from
the total ( d E / d x ) s calculated empirically~2). [Above 3
MeV/nucleon, eq. (1) can also be used to evaluate the
restricted energy loss rate]. The experimental data on
track registration in the two materials are superimposed
on the theoretical curves in the form of closed and
open circles and squares. Closed points indicate track
registration, open points indicate a lack of registration.
The circles correspond to data obtained by the authors,
the squares indicate data taken from Fleischer et a13).
Etching was carried out in 10 M N a O H solutions at
23 ° and 60°C for cellulose nitrate and polycarbonate
plastics, respectively. Although more measurements are
clearly desirable (particularly for the polycarbonate
plastic) the existing data suggest that a critical value
of the restricted energy loss rate can be chosen for
each of these materials. The thresholds for track
formation, RELcri, , for cellulose nitrate and poly-
carbonate plastics are found to be 1.1 x l03 and
3.3 × 103 MeV • cruZ/g, respectively.
In figs. 1 and 2, the data points for 0.1 MeV/nucleon
deuterons in cellulose nitrate, and 0.1 MeV/nucleon
alpha particles in polycarbonate resin fall below the
predicted region of track registration. However, since
the energy loss rates for the two ions are quite uncertain
at these low energies, it is not known if the discrepancy
is real. Also, there is evidence that the actual energies
are less than 0. l MeV/nucleon. This arises from the
 THE RESTRICTED ENERGY LOSS CRITERION 345

\ ,'-,,,

102- I I Illlrl ~1 IIIII1'~ I~LI[EIII

10 -] 10 ° 10 ~ 10 a 03 10 4
ENERGY/NUCLEON (MeV)

Fig. 1. Restricted energy loss rate, (dE/dx)oJ<loae'¢, as a function of energy per nucleon for a number of heavy ions in cellulose nitrate
(IadJ = 81.1 eV).

tendency to overestimate the length of very short
tracks since their size is near the resolution limit of the
optical microscope. At these low energies (approxi-
mately 0.05 MeV/nucleon) the principal mode of energy
loss is through nuclear collisions; therefore, the REL
model is no longer applicable. Further experimental
data for the registration of heavy, high energy ions is
required for an accurate determination of the para-
meters OJo and RELc, ..
The ~zC data in fig. I suggest that the transition in
energy between etchable and non-etchable track
damage is quite sharp. This was verified through an

10 5

E 10 4
o
6~-e

%
v
3

10 3

10 I I il l l l l ~ I I i i~Tr
10 -] 10 ° 101 10 2 10 3 10 4
ENERGY/NUCLEON (MeV)

Fig. 2. Restricted energy loss rate, (dE/dx)eo<lo3ev, as a function o f energy per nucleon for a n u m b e r o f heavy ions in Lexan
polycarbonate resin (laoj = 69.5 eV).
346
22
20
18
16
14
//,
F: 12
~L
Id- 10
8 (2 < z ~ 18). This similarity of predictions by the two
6
4
2 approach uses adjustable parameters to fit the existing
0 I I I I l I I I l
4 6 8 10 12 14 16 lib
~c-c, ~o~(~v~'----~)
Fig. 3. The average etch rate, 71, as a function of particle
average REL rate in N R D L - I cellulose nitrate plastic.
independent set of measurements using lzc, 160, and
4°Ar ions with energies up to 10 MeV/nucleon in
cellulose nitrate. The irradiated specimens were etched
in 10 M N a O H solution at 60°C for one minute. The
results appear in fig. 3. For large values of REL,
rT approaches a constant, saturation value. For low
values of R E / , r T very quickly decreases and at
REL = RELcrit, r T = r B.
3. Discussion
The REL criterion implies that if a dose (energy/unit
volume for the volume of the track) corresponding to
that from a heavy ion is deposited in a track detecting
material, a preferential etching of this region should
occur. The exact dimension, or the distribution of
energy within the latent track region is at present not
known. It is thought that the diameters of unetched
fission fragment tracks in a polycarbonate plastic are
probably no greater than about 100 A1). If the thres-
hold for charged particle track registration in cellulose
nitrate, 1.1 x l 0 3 MeV cm2/g, is assumed to be depo-
sited within this track volume, the average dose distri-
buted over this cylindrical volume is found to be appro-
ximately 2.5 × 10 7 rad. The track width of 100 A is for
a particle well above the threshold; for particles at the
threshold, the widths are probably narrower, resulting
in a dose > 2.5 × 10 7 rad.
This hypothesis was tested by irradiating cellulose
nitrate with fl-particles from a 4°Sr source in such a
manner that only a small area of the sample was
exposed while the remainder was shielded by a lead
E. V. B E N T O N A N D W. D. N I X
mask. After irradiating, the specimens were etched
at 23 °C in a 10 M NaOH solution for times comparable
to that needed to develop tracks of heavy ions. A dose
of about 4 × 10 7 rad resulted in a preferential etch rate
comparable to that from heavy ions. Similar effects
• 'oAr have also been observed with gamma rays.
The Primary Ionization, PI, and the Restricted
Energy Loss, REL, criteria give nearly identical predic-
tions as to track registration for the lighter ions
criteria is attributed primarily to the fact that the
functional dependence of eq. (1) and of the equation
for primary ionization on fl is very similar. Also, each
I I
experimental data. For heavier ions (z > 18) the REL
20 22 24 26 criterion predicts registration up to higher energies of
the incident particle. However, for high energies, the
predictions are quite sensitive to the R E L e r i t value
used. A 10% increase in the RELcrlt value for cellulose
nitrate lowers the maximum predicted energy for 56Fe
registration from 485 to 400 MeV/nucleon. The latter
value is predicted by the current P1 criterion
(I o = 2 eV). Both criteria agree well with the presently
available experimental data.
The PI and the REL criteria differ as to the mecha-
nisms of track formation, however. According to the
PI model, an etchable track is formed when the rate of
primary ionization (the average number of collisions
of the bombarding particle with the stopping electrons
per g/cm z that result in the ejection of an electron
from an atom) exceeds a critical value for that material.
The PI criterion neglects all the secondary and higher
order ionization produced by the ejected electrons
(f-rays). This is opposite to the view of the REL
model, and that of the work of Katz et al. 13) and
Pfohl et al.a 4). 1n highly radiation-sensitive polymers it is
reasonable to expect that the low energy f-rays which
have received sufficient energy to free them from their
parent atom will contribute to the total dose of the
latent track region. These low energy f-rays are
produced in copius numbers by heavy ions. Having
small kinetic energies and correspondingly small
ranges, these electrons undergo multiple scattering
throughout the latent track region, and deposit their
energy in and near the region of primary ionization.
For particles at the threshold of registration, this may
be an important contribution.
The REL offers an easy and a convenient way of
determining if the condition for registration is fulfilled.
It also allows assigment of absolute sensitivity in terms
of a microscopic dose to each of the polymeric track
detecting materials. Based on the REL model, a
 THE RESTRICTED ENERGY LOSS CRITERION
particle will produce a latent track over the extent of
its range where its R E L > RELcrit for that material.
The length of this region of the particle trajectory we
call Rreu, the registration range. The q u a n t i t y Rreg is a
very sensitive f u n c t i o n of z, varying approximately as
M z 2 for c a r b o n t h r o u g h M2"3"8 for iron. It has been
shown that in cellulose nitrate of u n i f o r m sensitivity,
charge (and possible mass) d e t e r m i n a t i o n can be
accomplished t h r o u g h the m e a s u r e m e n t of a par-
ticle's R~eg15).
N o t e added in proof" It has recently been reported that
in Lexan track-etching charactetistics vary slowly with
the age of the latent tracks.'16). In a current study we
discovered that in Lexan, preferential etching along the
particle trajectory can be dramatically incleased
t h r o u g h the irradiation of latent tracks with ultraviolet
radiation in the presence of oxygen. Thus to the para-
meters which influence track etching must be added
yet a n o t h e r category: the c o n d i t i o n s and the storage-
time prior to etching. The mechanisms of the U V e n h a n -
cement as well as the influence of storage conditions will
appeal in a f o r t h c o m i n g paper.
We wish to t h a n k Dr. H . H . H e c k m a n of the
University of California Lawrence R a d i a t i o n Labora-
tory for m a k i n g the Hilac irradiations possible. We are
also indebted to R. P H e n k e a n d M. M. Collver for
helpful suggestions a n d assistance d u r i n g the course
of this work.
347
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