Applied Radiation and Isotopes 118 (2016) 228231

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Applied Radiation and Isotopes

journal homepage: www.elsevier.com/locate/apradiso

A parameterization of the chemistry-normality dependence of bulk etch rate

in a CR-39 detector
crossmark
Mushtaq Abed Al-Jubbori
Department of Physics, College of Education for Pure Science, Mosul University, 41001 Mosul, Iraq

A R T I C L E I N F O A BS T RAC T

Keywords: An empirical relationship describing the bulk etch rate is formulated. The equation involves two free tting
Normality parameters, which reproduce the bulk etch rate for CR-39 by alpha particles at dierent normalities of the
Bulk etch rate etching solution. The values of the tting parameters were obtained from the experimental data. This
LengthDiameter (LD) method relationship is used to predict the bulk etch rate at dierent normalities.
Modeling
CR-39

1. Introduction by the accuracy of mass measurements. The other method used to

Solid state nuclear track detectors (SSNTDs) have applications in
nuclear physics, cosmic ray physics, space physics, particle accelerator
physics, archeology, geology, medicine and biology (Hiroko and
Nobuhito, 2000; Stejny et al., 2000; Rana et al., 2000; Hermsdorf
and Hunger, 2009; Al-Jubbori, 2013). One of the basic parameters
required for the use of an SSNTD is the bulk etch rate, VB (Ditlov et al.,
2008; Awad et al., 2009; Azooz and Al-Jubbori, 2016). This is dened
as the rate at which an etchant erodes the target material in a general
direction (Azooz et al., 2012a, 2012b; Hermsdorf, 2012). There are
many methods to determine the bulk etch rate for SSNTDs. The most
straight forward is the measurement of the eroded thickness, h ,
during the etching process of a detector surface in a specic interval of
time, t , then calculating VB (Durrani, 1987) as:
1 h
VB =
2 t
The factor 2 above takes account of the removal of the thickness
from both sides of the at surfaces of a detector sheet. Another method
relies on measuring the detector mass before and after etching. Based
on the mass dierence and the known density of the detector, it is
possible to determine the thickness of the removed layer and in turn
VB. This method is sometimes called the gravimetric method and it
determine VB (Malik et al.,2002) by:
m times, detectors were exposed to alpha particles from a 241Am source
VB =
2At
where m is mass dierence, A the etched surface area, the density of
the detector and t is the etching time. However, this method is limited
measure VB is the LD method, which is based on studying the
relationship between the tracks length L and diameter D for irradiated
detectors, and using the relation (Manzoor et al., 2007):
D2 4L2
VB = 1 + 1+
4tL D 2 (3)
The use of digital image processing can result in improvement of
measurement accuracies of both methods. Such technique is employed
in this work and results from both methods are compared.
2. Experiments
For the removed thickness measurement method, unirradiated
1010 mm, 200 m thick CR-39 detectors made by Page Moldings
(Pershore, UK). The detector was etched each 10 min, and a digital
(1) image after each etching was obtained and used to obtain the
remaining detector thickness. Typical image is shown in Fig. 1. The
images were analyzed to obtain the remaining detector thickness by
converting digital pixels to micron thickness. The value of VB following
each etching process was obtained from dening sharp boundaries
between contrasting picture regions derived from color contours
calculations.
In order to obtain track longitudinal proles and track diameters at
dierent etching chemistry-normality (degree of acidity) and etching
(2) with 3.2 MeV energy. This energy represents the middle of the energy
range where such detectors are typically used. The exposure system
involves narrow collimation in order to obtain an almost perpendicular

E-mail address: mushtaq_phy8@yahoo.com.

http://dx.doi.org/10.1016/j.apradiso.2016.09.022
Received 17 May 2016; Received in revised form 19 September 2016; Accepted 19 September 2016
Available online 20 September 2016
0969-8043/ 2016 Elsevier Ltd. All rights reserved.
M.A. Al-Jubbori Applied Radiation and Isotopes 118 (2016) 228231

Fig. 1. Digital image of the lateral view of an etched unirradiated detector.

incidence angle. The detectors are sharply broken at the small 1 mm2
exposed area. The etching was carried out in 70 C NaOH solutions, at
normality of 6.25, 7.5, 8.0, 8.5 and 9.0 N. The detector was etched for
10 min and then digitally photographed by a digital USB camera
(OPTICA 4083. B5) attached to OPTIKA B-193 microscope. Typical
images are shown in Fig. 2(a) and (b), for track length and diameter,
respectively. The etching process was repeated over several 15 min
periods, and digital images for the longitudinal and lateral develop-
ment of the tracks were recorded. A special MATLAB image processing
software was used to performs image-brightness contour analysis to
dene the track boundaries. The outermost well dened contour
dened the track dimension, while the maximum contour line uctua-
tions amplitude along the contour dened the error in measurement.
Example of such measurements for the radius is shown in Fig. 2(c),
which suggests a measurement error of about 1%. Errors values are
aected by image quality. In most cases, errors did not exceed 3%.

3. Results and discussions Fig. 2. Digital images of: (a) track length, (b) track diameter at 1 h for E=3.2 MeV, (c)
contour edge diameter.
Thickness results from the rst method discussed above are used to
calculate VB using Eq. (1). The bulk etch rate was determined by 25
o
performing a linear t of h versus t. The results are presented in Fig. 3 y=2.7321x -0.2589 for N=6.25 T=70 C
which shows the experimental data and linear t results at solution
y=3.9526x -0.20661 for N=7.5
normality of 6.25, 7.5, 8.0, 8.5 and 9.0 N respectively. Values of VB
Removed Layer Thickness h ( m)

20
calculated from Eq. (1) are shown in Table 1. y=4.3214x -0.1071 for N=8.0
Results of measurements of L and D versus etching time are shown y=4.821x -0.4464 for N=8.5
in Fig. 4. Values of L prior to track length saturation together with the y=5.802x -0.359 for N=9.0
15
corresponding D values were substituted in Eq. (3) to calculate VB. The
results related to the time development of VB are presented in Fig. 4(c).
Results in this gure indicate that there are no signicant variations of
VB with the exception of those related to the highest normality. The 10
time averaged results of all VB values are presented in the third column
of Table 1. It may be worth mentioning here that the track saturation
length in Fig. 4(a) is independent of etching normality. This gives 5
further credibility to the measurement technique used. It must be
emphasized however that the accuracies of the removed layer results
are better than the corresponding LD method results due to the
0
combined errors in the latter (Hermsdorf et al., 2007; Azooz and Al- 0 0.5 1 1.5 2 2.5 3
Jubbori, 2013). Etching Time (h)
The track etch rate, VT, was determined for the time-dependent
Fig. 3. Relationship between removed layer thickness and etching time.
track length, L, the relationship: VT = dL / dt + VB .
This quantity can be derived from measured time evolution of the

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M.A. Al-Jubbori Applied Radiation and Isotopes 118 (2016) 228231

Table 1 12
Comparison of VB measured in two methods.

Normality (m h1) Bulk Etch Rate VB 10

Removed Thickness Method LD Method o

T=70 C
6.25 1.37 0.02 1.28 0.05
8
7.5 1.98 0.02 1.80 0.05
8.0 2.16 0.03 2.07 0.07

L ( m)
8.5 2.41 0.03 2.57 0.09 6
9.0 2.90 0.03 3.02 0.09

4
track length (Fig. 4(a)) by calculation of the rst derivation of L(t).
N=6.25
Fig. 5 shows the track etch rate obtained by numerical dierentiation
N=7.50
procedures. 2
N=8.00
Fig. 6 shows the results of track saturation time, tsat , relation to N=8.50
normality as derived from Fig. 4(a). These data are well described by N=9.00
the exponential form in the relationship: 0
0 1 2 3 4 5 6
tsat = a1 ea2 N + a3 Etching Time (h)
(4)

The tting parameters values a1 = 179.648 h, a2 = 0.5904 , and

12
a3 = 0.0018 h. In Fig. 6 the results of t are compared with those of o
Hermsdorf and Mahmood (2013), described the saturation time by T=70 C
tsat = (1.127 + 1.244. E + 0.237. E2 )/VB . 10
In order to develop an empirical relationship between the bulk etch
rate and normality, the VB data from this work were combined with
other data at a lower normality range published by Gruhn et al., (1980) 8
and Ahn and Kilee, (2005), and plotted against etching solution
normality on Fig. 7. In the absence of a detailed theory describing
D ( m)

the eect of solution concentration on bulk etching rate, it may be 6

useful to attempt to propose some empirical relationship that properly
describes the experimental data. Any empirical equation that describes
4
the experimental results in Fig. 7 must produce numerically acceptable
convergent t in the range of the experimental data considered. This is N=6.25
N=7.50
usually an easy task and a polynomial of some degree can result is such 2
N=8.00
t. The relationship must also describe the behavior at zero and very
N=8.50
high concentrations. The third is that it is also desirable to have an N=9.00
empirical equation with a minimum number of free tting parameters. 0
0 1 2 3 4 5 6
Keeping in mind that the reaction between the etching solution and the Etching Time (h)
detector material is a rst-order irreversible chemical reaction, which
usually assumes an exponential behavior, the following equation is
proposed 3.5
o N=6.25
VB = a (e bN 1) (5) T=70 C
N=7.50
N=8.00
with a and b as two free tting parameters. This equation produces very 3
N=8.50
high bulk etch rate at very high concentration, which corresponds to N=9.00
very small track saturation time. This is consistent with the fact that
highly concentrated sodium potassium and calcium hydroxides solu- 2.5
VB ( m/h)

tion can vigorously attack most organic materials. The equation also
gives zero bulk etch rate at zero concentration (distilled water), which
corresponds to innite track saturation time. The equation produced
2
the best t of the data with minimum number of free tting parameters
(two only), with over 95% condence level t. From purely tting
theory point of view, this is accepted to be better than any polynomial
t which involves three parameters at least. The tted values of the two 1.5
parameters above are a = 0.478 m/h , b = 0.2151.
Experimental data and t results to Eq. (5) are also compared with
two empirical relation proposed by Fromm et al. (1991) and Somogyi 1
0 0.5 1 1.5 2 2.5 3 3.5
and Hunyadi (1979) which described the VB dependence upon both
Etching Time (h)
concentration C and absolute temperature T in forms:
VB = 1.276 exp(0.828C + 0.049T 0.002CT 17.624) (6)
Fig. 4. Time development of track dimensions at dierent etching normality: (a) track
length, (b) track diameter, (c) bulk etch rate calculated from data in (a) and (b) using Eq.
VB = fB C nB e / kT (7) (3).

where T is the temperature in K, C is the concentration of the etchant in

the unit of normality and k is the Boltzmann's constant. The constants

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M.A. Al-Jubbori Applied Radiation and Isotopes 118 (2016) 228231

20 fB , nB and the activation energy were obtained from tting proce-

T=70 oC N=6.25
dures as fB = 0.0318m/h , nB = 2.0421 and / k = 1.0019 K. These corre-
18 N=7.50
spond to activation energy of 8.6414 105 eV/molecule.
N=8.00
16 Substitution the temperature value of 70 C gives the normality
N=8.50
N=9.00 dependence of VB shown as blue and red dash line in Fig. 7. It is clear
14 that the result of t using Eqs. (5) and (7) produced results which are
12
more consistent with experimental data.
VT ( m/h)

10 4. Conclusions

8 The use of digital image processing to study the bulk etch rate of
6
CR-39 nuclear track detector resulted in improved accuracy in measur-
VT=VB ing this quantity using two well-known methods. These methods are
4 the removed layer method and the LD method. The results of both
methods were in good a agreement. The study of the eect of etching
2
solution concentration on track saturation time indicated an exponen-
0 tial behavior, which can be described by a simple relationship, Eq. (5).
0 1 2 3 4 5 6
Etching Time (h)
Acknowledgment
Fig. 5. Track etch rate at ve etching solution concentrations.
The author would like to thank Prof. Dr. Aassim A. Azooz of the
5.5 Department of Physics, College of Science, Mosul University for useful
data discussions.
5 Fit
Hermsdorf and Mahmood 2013
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