540 Nuclear Instruments and Methods in Physics Research 220 (1984) 540-546

North-Holland, Amsterdam

DETERMINATION OF CRITICAL ANGLES OF ETCHING AND TRACK REGISTRATION

EFFICIENCIES OF TRACK DETECTORS

HAMEED AHMED KHAN

Nuclear Engineering Division, Pakistan Institute of Nuclear Science and Technology (P1NSTECH), P.O. Nilore, Rawalpindi, Pakistan

Received 25 May 1983

The critical angles of etching and the track registration efficiencies of different types of solid state nuclear track detectors
(SSNTD) have been determined. An extensive use of the scanning electron microscope (SEM) has been made in this regard. From the
pictorial observations, numerical values of track parameters such as (a) 8, the cone angles, (b) 8c, the critical angles of etching, and (c)
v/, the track registration efficiency (in 2~r-geometry) were obtained. A decrease in the critical angles of etching and an increase in
particle registration efficiency with the increasing value of (a) restricted energy loss (REL), and (b) (Zeff/fl) 2 o f the incident particles
have been observed. The results are expected to be useful in experiments carried out for the quantitative study of the emission of
charged particles in nuclear reactions and for the determination of reaction cross sections.

1. Introduction
Experience shows that the critical angle of etching *
is an important parameter in the field of solid state
nuclear track detection (SSNTD) [1]. It is of great
significance when we employ track detectors for
quantitative studies of the emission of different types of
charged particles in nuclear reactions. The parameter is
particularly useful for the determination of reaction
cross sections and the angular correlations using planar
SSNTDs [2]. Some experiments have been carried out
for the determination of critical angles of etching of
some glass and plastic track detectors for fission frag-
ments [1-4]. Very limited work has been reported con-
cerning the 0c measurements for ions other than fission
fragments [4].
Hostaphan and CR-39 are relatively new plastic track
detectors. CR-39 has been found to be sensitive to both
heavy and light charged particles [5-8]. Although some
work has been reported on the determination of the
critical angle of etching of CR-39 [4], no such measure-
ments have, apparently, been m a d e regarding
Hostaphan. Moreover, a lot more work is yet to be done
to find the critical angles of etching of the conventional
type of SSNTDs for various charged particles with
different energies. This paper summarizes the experi-
ments carried out at P I N S T E C H in order to determine
* It is the angle between the detector surface and trajectory of
the incident charged particle, which separates the "etchable"
and "non-etchable" angular intervals. Exposures carried out
below this critical angle will not produce etchable latent
damage trails.
critical angles of etching for both light and heavy charged
particles, having a wide spectrum of energies. The 0r
values so obtained have been used to calculate the track
registration and development efficiencies.
2. Experimental details
Two types of experiments were carried out for the
determination of critical angles of etching.
2.1. Direct measurements
In this method a number of small pieces of a particu-
lar type of detector was positioned on an aluminium
backing so that the surfaces of the detectors were sub-
tending different angles with respect to the incoming
beam of charged particles. In certain cases, the particles
were decelerated to some pre-determined energies by
using a wedge of degraders. The tracks in the exposed
detectors were developed by using appropriate etchants.
Careful measurements were made regarding the track
densities and the etch-pit dimensions at various angles
of incidence. Observations were made to find out the
angular interval in which the tracks fail to produce
etchable latent damage trails. The angular interval was
finally narrowed down with a view to determine the
exact value of the critical angle of etching. The critical
angles of etching of CR-39 plastic track detector for
protons and alpha particles having energies E~< 10
M e V / u were determined by using this method. The
technique was also employed for 8c measurements con-
cerning fission fragments.

0167-5087/84/$03.00 Elsevier Science Publishers B.V.

(North-Holland Physics Publishing Division)
 H.A. Khan / Critical angles of etching 541

P
2.2. Use of scanning electron microscopy (SEM)

Secondly, an extensive use of the scanning electron

microscopy (SEM) was made. Here, energetic ions were
allowed to fall perpendicularly to a particular type of
detector (or on a stack of detectors when dealing with
highly energetic, light, charged particles). The exposed
detectors were etched and the etch pit channels were
broken apart so that their profiles could be studied
under a scanning electron microscope (SEM). Using this
technique, the cone angles of the etched channels were
experimentally determined. Knowing that the cone an-
gle is twice the critical angle of etching, accurate values
of the critical angles were obtained. The registration
efficiency was calculated by using the following equa-

Fig. 2. A photomicrograph showing the cutaway sections of

etched channels in a phosphate #ass. The detector was etched
in 10N NaOH [kept at (60+ 1)C] for 1 h.

Fig. 1. A set of three SEM photomicrographs showing the

profiles (side views or cutaway sections) of etch pits due to (a)
12.5 MeV/u 84Kr, (b) 4.7 MeV/u 136Xe, and (c) 10.0 MeV/u Fig. 3. Cutaway section or a side view of two etched channels
23Su ions in soda lime glass track detectors. The etching was due to 7.5 MeV/u 238U ions in a vitreous silica etched in 48%
carried out in 48% HF (room temperature) for 20 s. HF.
 542 H.A. Khan / Critical angles of etching
tion [2,3]:
*/(efficiency in 2~r-geometry) = 1 - sin 0c. (1)
Some details of the charged particles employed in
the present studies have been given in table 1.
After the exposure, the detectors were etched as
follows:
Hostaphan 33% 6N NaOH + 33% H20 + 33%
CH3OH, at (40 + 1)C
CR-39 6N NaOH, (70 + 1)C
Muscovite
mica 48% HF, room temperature (about 22C)
Soda lime
glass 48% HF, room temperature (about 22C)
Phosphate
glass 10 N NaOH, (50 + 1)C
Lexan 6N NaOH, (50 + 1)C
Makrofol N 6N NaOH, (50 + 1)C
Makrofol E 6N NaOH, (50 + 1)C.
3. Results and discussion
Fig. 1 is a collection of photomicrographs showing
the side views of etched channels in soda lime glass. The
three channels were produced by (a) 12.5 MeV/u S4Kr,
(b) 4.7 MeV/u 136Xe, and (c) 10.0 MeV/u 23Su ions.
The detectors were etched simultaneously in 48% HF at
room temperature (about 22C) for 20 s. Comparison of
figs. l a and b clearly indicates a decrease in cone angle
with increasing Z-number of the incident particle.
The photomicrographs shown in fig. 1 are some
typical examples. In order to obtain representative num-
bers for the cone angles and the critical angles of
etching, a large number of such events was scanned and
photographed, and them the physical measurements of
the cone angles were carried out. Experience shows that
the exact value of the cone angle is obtained when the
break is such that it passes through the vertex of the
etched cone. In such a situation, the cone angle so
obtained is found to have the minimum possible value.
Due to these considerations, etched channels were
analysed and the minimum value of the cone angles
from their distributions were selected as the representa-
tive angle. Following the above described procedure,
values of cone angles and of the critical angles of
etching were obtained for a variety of ions in the soda
lime glass detector. The results as summarized in table 2
indicate a systematic decrease in the cone angle and the
critical angle of etching with increasing Z-number of the
incident ion. It is interesting to note that very little
change in 8 and 0 is obtained for a particular ion
having different energy values.
Profiles of four etched channels due to 10.0 MeV/u
238U ions in a phosphate glass are shown in fig. 2.
Comparison of these channels with those shown in fig.
lc indicates a significant difference between the track
registration and etching properties of these two types of
glasses. The results obtained for the phosphate glass
have been summarized in table 3. Measurements were
also made on a vitreous quartz glass. The results (fig. 3
and table 4) indicate that the track registration proper-
ties of quartz glass lie in between those of a phosphate
glass and a soda lime glass. The values obtained here
(by using a combination of direct method and SEM
analysis) are found to be quite different from those
determined previously for another type of vitreous quartz
[2]. The results indicate that the efficiencies of quartz
glasses may differ quite a lot. Therefore, each quartz
glass has to be calibrated separately before using it in
quantitative work.
The importance of the minimum cone angle for the
determination of 8c is once again emphasized here. In
fig. 3, profiles of two etched channels due to 7.5 MeV/u
23Su ions are shown. It is quite evident from the mea-
surement of the angles of cone 'a' and cone ' b ' that
although the parameters of the particles producing these
two cones are the same, widely different values (25030 ,
and 32045 ') of the cone angles are obtained for cone 'a'
and cone ' b ' respectively. The values of 8 and 0 quoted
in table 4 were compiled from the minimum values
obtained for the cone angles.
Experiments concerning Muscovite mica yielded in-
teresting results. The cone angles determined from the
SEM analysis of the cutaway-etched channels were
found to have very small values. The etched channels
due to 23SU and 136Xeetc. were almost cylindrical with
very little conical structure. However, the etched chan-
nels due to fission fragments, S4Kr, and lighter ions
(such as 32S) were found to have a clear cut conical
structure for which the determination of 8 and 8 was
comparatively easier. Fig. 4 is a set of two SEM photo-
micrographs of etched channels due to fission fragments
showing (a) the top view of the openings, and (b) the
track openings and the cross-sectional views. A visual
comparison of the two top views (at the upper and
lower ends of the cutaway sections of the etched chan-
nels) of fig. 4b clearly gives a feeling of the magnitude
of tapering of the fission fragment etched channels. The
results have been summarized in table 5. The presently
obtained results for fission fragments are comparable
with the ones obtained previously by using the direct
method of 0 determination [2].
The recently introduced detector of CR-39, because
of some of its unique properties, has become very
popular in the field of solid state nuclear track detec-
tion. Due to the great importance of this plastic, 0c
measurements were performed with almost all the avail-
able charged particles. The results of these measure-
ments along with the track registration efficiency values
 H.A. Khan / Critical angles of etching 543

Table 1
Details of the charged particles employed in the present work
# #
Charged Energy/nucleon Source/accelerator
particles [MeV/u]
23SU 10.0
7.5
UNILAC, GSI, Darmstadt,
West Germany
r , # 4
1.4
136Xe 8.5
4.7
s4 Kr 12.5
0 t # # ,
4.6

32S 3.2 Tandem accelerator,

19F 5.5 MPI, Heidelberg,
West Germany

160 107 CERN-SC, Geneva,

1So 86 Switzerland
12C 86

4He 10 Nuffield cyclotron,

Protons 10 Birmingham University,
England

Fission spontaneous 252C f-spontaneous

Fig. 4. A set of two photomicrographs showing (a) the top view,
fragments fission spectrum fission source
and (b) the top and side views (of a section) of etched channels
( - 1 MeV/u)
due to collimated fission fragments in a Muscovite mica track
detector.

Table 2
Cone angles and the critical angles of etching of a soda-lime glass track detector a)

Charged Energy/nucleon Minimum value of Oc

particle [MeV/u] cone angle, 8
238U 10.0 58 30' 29 15'
238U 1.4 60 45' 30 23'
136Xe 4.7 70 15' 35 08'
Fission fragments spontaneous fission spectrum 72 00' 36 00'
( - 1 MeV/u)
S4Kr 12.5 76 00' 38 00'
S4Kr 4.6 76 30' 38 15'

a) Obtained from Wenzel Glass, Berlin, West Germany.

Table 3
Cone angles and the critical angles of etching of a phosphate glass a)

Charged Energy/nucleon Minimum value 0

particle [MeV/u] of cone angle,
23Su 7.5 4 30' 2 15'
23Su 10.0 4 45' 2 23'
136Xe 8.5 6 45' 3 23'
Fission fragments spontaneous fission spectrum 7 30' 3 45'
( - 1 MeV/u)
S4Kr 12.5 8 30' 4 15'
S4Kr 4.6 8 00' 4 00'

a) Composition: 68.45[ P2Os; 13.65[ ZnO; 85[ A1203; 7.95[ B203; 2.15[ SiO2; obtained from Leitz GmbH, Postfach 2020, Braunfelser
Strasse, Wetzlar, West Germany.
 544 H.A. Khan / Critical angles of etching

Table 4
C o n e angles a n d the critical angles of e t c h i n g o f vitreous q u a r t z glass d e t e c t o r s a)

Charged Energy/nucleon M i n i m u m value of

particle [MeV/u] c o n e angle,
23Su 7.5 24 30' 12 15'
23Su 10.0 24 45' 12 23'
136Xe 8.5 28 00' 14000 ,
Fission fragments s p o n t a n e o u s fission s p e c t r u m 29 30' 14 45'
( ~ 1 MeV/u)
S4Kr 12.5 31 30' 15 45'
S4Kr 4.6 32 0 0 ' 16000 ,

a) O b t a i n e d f r o m C h a n c e B r o t h e r s Limited, E n g l a n d .

Table 5
C o n e angles a n d the critical angles of e t c h i n g o f a m u s c o v i t e m i c a t r a c k d e t e c t o r a)

Charged Energy/nucleon M i n i m u m value of 0c

particle [MeV/u] c o n e angle, ;~
23Su 7.5 2 00' 1 00'
23Su 10.0 2 30' 1 15'
136Xe 8.5 4 30' 2 15'
Fission fragments s p o n t a n e o u s fission s p e c t r u m 7 30' 3 45'
( - 1 MeV/u)
S4Kr 12.5 8 15' 4 08'
SaKr 4.6 8 00' 4 00'
32S 3.2 20 30' 10 15'

a~ O b t a i n e d f r o m S c h e r b a n d Schwer, Berlin, W e s t G e r m a n y .

Table 6
C o n e angles, the critical angles o f e t c h i n g a n d the t r a c k r e g i s t r a t i o n efficiencies (in 2~r-geometry e x p o s u r e s ) o f C R - 3 9 plastic t r a c k
d e t e c t o r s a)

Charged Energy/nucleon Cone Critical a n g l e Track registration

p a r t i c l e b) [MeV/u] angle, 8 o f e t c h i n g , 0c efficiency, (7/) [%]
238U ions [1] 10.0 1 48' 54' 98.4
2 s p b ions [1] 8.5 2 24' 1 12' 97.9
8 4 K r ions [1] 12.5 2 36' 1 18' 97.7
F i s s i o n f r a g m e n t s [1] s p o n t a e o u s fission of 152 C f 30 00' 15 00' 75.1
( - 1 MeV)
1 8 0 ions [2] 66.4 54 0 0 ' 27 0 0 ' 54.6
34.3 53 24' 26 4 2 ' 55.0
13.6 39 12' 19 36' 66.5
1 6 0 ions [2] 66.9 55 48' 27 54' 53.2
36.6 52 4 8 ' 26 24' 55.5
6.6 25 0 0 ' 12 30' 78.4
4.6 18 0 0 ' 9 00' 84.4
1 ions [2] 86.0 107 00' 53 30' 19.6
32.2 53 00' 26 30' 55.4
8.5 39 0 0 ' 19 30' 66.6
Alpha 10.0 56 4 8 ' 28 24' 52.4
particles [3] 4.7 52 0 0 ' 26 0 0 ' 56.2
1.8 51 36' 25 48' 56.5
0.6 32 4 8 ' 16 24' 71.8
0.23 12 48' 6 24' 88.9
P r o t o n s [4] 10.0 122 00' 61 00' 12.5
7.8 116 00' 58 00' 15.2
4.0 96 00' 48 00' 25.7
1.2 54 0 0 ' 27 0 0 ' 54.6

~) O b t a i n e d f r o m H o m a l i t e C o r p o r a t i o n , W i l m i n g t o n , D e l a w a r e , U S A .
b) E t c h i n g c o n d i t i o n s : 6 N N a O H , (70_+ 1)C: [1] 1 h; [2] 8 h, [3] 16 h; [4] 32 h.
 H.A. Khan / Critical angles of etching 545

Table 7
The cone angles, the critical angles of etching and the track registration efficiencies of hostaphan a) plastic for different charged
particles
Charged Energy/nucleon Cone Critical angle Track registration
particle [MeV/u] angle, 8 of etching, 0 efficiency b), ~1[%]
Z3Su 10.0 2 30' 1 15' 97.8
2spb 8.5 3 20' 1 40' 97.1
S4Kr 12.5 4 20' 2 10' 96.2
Fission fragments - 1 5 30' 2 45' 95.2
1So 86.0 130 00' 65 00' 9.4
160 107.0 152 30' 76 15' 2.9
12C 86.0 165 00' 82 30' 0.9

~) Obtained from Kalle, Wiesbaden, West Germany.

b) As calculated for thin sources in 2~r-geometry exposures.
Table 8
Critical angles of etching and track registration efficiencies a) of some plastic track detectors

Detector Charged Energy/nucleon Critical angle Track registration

particle [MeV/u] of etching, 0 efficiency ~), rl [%]
Lexan [1] Fission From 252Cf spontaneous 2 15' 96.1
fragments fission source ( - 1 M e V / u )
180 66.4 34 30' 43.4
160 107.0 38 45' 37.4
12C 86.0 64 30' 9.7

M akrofol-N b) Fission From 252Cf spontaneous 3 15' 94.3

fragments fission source ( - 1 M e V / u )
160 107.0 38 00' 38.4

Makrofol-E b) Fission From 251Cf spontaneous 2 30' 95.6

fragments fission source ( - 1 M e V / u )
160 107.0 31 00' 48.5
12C 86.0 59 15' 14.1

=') Calculated for thin sources in 2*r-geometry exposures.

b) Obtained from Bayer Chemicals Ltd., Leverkusen, West Germany.
35

b.I
IM r i T Oo [ DETECTOR: CR-~91 HOMALITE ]
boo ~g ,m, ~o
I00
D v tU
%o

(.9
z_
-i-
,.)
F-
g
tLI ao ~
t=,.
0
~I, ,5 =,
(.9
Z
< lt2
.J
o <[
o_ 5o ~
V- P_
o
5O

' ~ ~ i ~ 40 L i I I i I I h j . . . . . 45
104
~o io
RESTICTED ENERGY LOSS (MeV cruZ/gin)
(Zef f / ~])= OF THE CHARGED PARTICLES REL ((.~o " 2 0 0 eV)

Fig. 5. Variation of critical angle of etching and the track registration efficiency (in 2~r-geometry) of CR-39 as a function of (a)
2
Zcff/fl 2 , and (b) restricted energy loss (REL), of a variety of charged particles having a wide spectrum of energies.
546 H.A. Khan / Critical angles of etching
(for 2~r-geometry exposures) have been summed up in
table 6. It is interesting to note that even high energy
protons manage to produce etchable latent damage trails
with appreciably high efficiency. Similarly, 12C and 160
ions having energies in the intermediate energy range do
produce etchable damage - a feat that could not be
matched by the previously existing track detectors.
Hostaphan plastic is also a relatively new detector.
Very limited use of this detector has been until now.
Our early experience indicated that the detector pos-
sessed some very useful properties. Encouraged by these
early results, it was decided to carry out systematic
track registration studies of Hostaphan. Almost all the
critical angle measurement work described here was
performed using scanning electron microscopy. Since
the detector is not brittle (as CR-39) the profile studies
were found to be relatively difficult. The etched detec-
tors were at first immersed in liquid nitrogen for appre-
ciably long times and then they were suddenly taken out
and broken apart for studying the side views of the
etched channels. In many cases the breaking action was
not very smooth and the resulting sections were found
to have undergone some sort of twisting, which caused
distortion of the etched channel profiles. Such samples
were rejected for SEM studies. The results shown in
table 7 indicate that the track registration efficiency of
the Hostaphan detector for fission fragments and heavier
ions is comparable to that of CR-39. However, CR-39
has a much higher efficiency for ions such as lSO, 160,
12C etc.
The values of critical angles and the efficiencies of
(a) Lexan, (b) Makrofol N, and (c) Makrofol E for
fission fragments are given in table 8.
With a view to constructing a common curve for
different particles having a wide spectrum of energies,
the critical angles of the CR-39 detector were plotted as
a function of (a) Z2ff/fl 2, and (b) restricted energy loss
(REL) of the ion. Figs. 5a and 5b show the results thus
obtained. It is interesting to note that although the data
obtained for a variety of particles were employed in the
construction of these figures, the points plotted traced
out well defined single curves for each parameter. Both
figures indicate a gradual decrease in the critical angles
of etching for increasing values of the parameters z~./,8
2 2
and REL. The error bars given in fig. 5a represent only
statistical errors. For the sake of comparison, the depen-
dence of the track registration efficiency on Z2~ff/fl 2 and
REL has also been drawn in figs. 5a and 5b. The
variation of efficiency shows an increase with increasing
values of the above two particle parameters.
4. Conclusions
The following conclusions have been drawn from the
above results:
(1) In general, the critical angle of etching of a
particular detector decreases (or the track registration
efficiency increases) with increasing values of the (a)
charge, (b) Z2~,/fl 2, and (c) restricted energy loss (REL)
of the incident ions.
(2) Among the detectors investigated here, CR-39
plastic and the soda lime glass detectors are found to be
the most sensitive and the least sensitive track detectors,
respectively.
(3) The critical angles of etching of CR-39, Musco-
vite mica, Lexan, Makrofol N, Makrofol E and phos-
phate glass for heavy charged particles (such as 238U
ions, fission fragments, and 136Xe ions) have compara-
ble values.
(4) The difference in the values of 0c and track
registration efficiencies of the presently investigated
track detectors increases remarkably for light ions such
as 84Kr, 32S, 19F, 160, 180, lZc, 4He, etc.
(5) The heavy ion track registration efficiency of
Hostaphan plastic (a relatively new track detector) is
comparable to that of Muscovite mica and phosphate
glass. However, the detector is very inefficient for the
registration of lighter ions.
(6) Study of the etched channel profiles by using a
scanning electron microscope is a useful method for the
determination of critical angles of etching.
It is a pleasure to thank all the colleagues at (a)
UNILAC, GSI, Darmstadt, (b) Tandem Accelerator,
MPI, Heidelberg, (c) CERN-SC, Geneva, and (d) NUF-
FIELD Cyclotron, Birmingham University, for their
invaluable help during the exposure of the detectors and
for many useful discussions. Thanks are also due to the
members of the SSNTD Group (PINSTECH) for their
help in the analysis of some of the samples. The finan-
cial help of the Alexander von Humboldt (AVH)
Foundation during my stay at Kernchemie, Philipps
Universit/it (Marburg, West Germany), is also gratefully
acknowledged. I am also grateful to Dr. Naeem Ahmad
Khan and Mr. K.M. Akhtar for their encouragement
and interest in the present work.
References
[1] R.L. Fleischer, P.B. Price and R.M. Walker, Nuclear tracks
in solids: principles and applications (University of Cali-
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[3] Hameed A. Khan, Nucl. Instr. and Meth. 173 (1980) 43.
[4] E.V. Benton and N.M. Ceglio, Proc. 10th Int. Conf. on
Solid state nuclear track detectors, [,yon (1979) p. 747.
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Meth. 153 (1978) 457.
[6] H.B. Luck, Nucl. Instr. and Meth. 198 (1982) 611.
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