Applied

Radiation and
Isotopes
PERGAMON Applied Radiation and Isotopes 51 (1999) 209215

Determination of uranium and thorium contents inside

dierent materials using track detectors and mean critical
anglesp
M.A. Misdaq a, *, A. Bakhchi a, A. Ktata a, A. Merzouki a, N. Youbi b
a
Nuclear Physics and Techniques Laboratory, Faculty of Sciences Semlalia, B.P.S 15, University Cadi Ayyad, Marrakech, Morocco
b
Laboratory of Petrology, Faculty of Sciences Semlalia, B.P.S 15, University Cadi Ayyad, Marrakech, Morocco
Received 6 March 1998; received in revised form 26 October 1998

Abstract

The critical angles of the CR-39 (yc) and LR-115 type II (yc 0 ) solid state nuclear track detectors (SSNTD) for
detecting a-particles emitted by the uranium and thorium series have been evaluated by calculating the
corresponding ranges of the emitted a-particles in dierent material samples and in the SSNTD studied. The
inuence of the emitted a-particles initial and residual energies on the critical angles of the SSNTD studied has been
investigated. The uranium and thorium contents of dierent geological samples have been evaluated by exploiting
data obtained for the critical angles of the CR-39 and LR-115 type II solid state nuclear track detectors and
measuring the corresponding densities of tracks. # 1999 Elsevier Science Ltd. All rights reserved.

1. Introduction (Jurado Vargas et al., 1997), radiochemical separations

Many authors have studied the inuence of the etch-
ing conditions and incident energies of a-particles on
the CR-39 and LR-115 type II solid state nuclear track
detectors critical angles of etching (Somogyi, 1980;
Membrey et al., 1993). Others have measured the criti-
cal angles for the CR-39 and LR-115 type II SSNTD
by using monoenergetic beams of a-particles (Jonsson,
1981; Barillon et al., 1995). The critical angle of the
CR-39 SSNTD for a-particles emitted by radon
(222 Rn) and its decay products in air have been deter-
mined by using a software programme which is based
on the BetheBloch's expression for the stopping
power for heavy charged particles in a medium and on
Monte Carlo simulations (Nikezic' et al., 1996).
Uranium and thorium contents have been measured in
various material samples using alpha spectrometry
p
This work was partially realized under a research contract
with the CNESTEN-Rabat.
* Corresponding author. Tel.: +212-4-434-649; fax: +212-
4-436-769; e-mail: ucadp@cybernet.net.ma.
(Herranz et al., 1997) and extraction chromatography
with anion exchange and alpha spectroscopy
(Goldstein et al., 1997).
The solid state nuclear track detector (SSNTD) tech-
nique was utilized for uranium contents determination
in dierent geological samples (Samad Baig et al.,
1983; Jojo et al., 1994; Misdaq and Satif, 1995; Satif
and Misdaq, 1995).
In this work, we describe a method based on deter-
mining the residual energies of a-particles emitted at
dierent points inside dierent material samples on
which CR-39 and LR-115 type II lms have been
placed, for evaluating the critical angles of these con-
sidered SSNTD. We also develop a new technique
based on exploiting data obtained for the critical
angles of the considered SSNTD and measuring the
densities of tracks per unit exposure time registered on
these detectors for determining the uranium and thor-
ium contents of the material samples studied. The rel-
evant ranges of a-particles emitted by the uranium and
thorium series, in the considered materials and SSNTD
utilized, were calculated by means of a TRIM pro-
gramme (Biersack and Ziegler, 1992).

0969-8043/99/$ - see front matter # 1999 Elsevier Science Ltd. All rights reserved.
PII: S 0 9 6 9 - 8 0 4 3 ( 9 8 ) 0 0 1 9 0 - 0
210 M.A. Misdaq et al. / Applied Radiation and Isotopes 51 (1999) 209215

2. Method of study holes. The CR-39 SSNTD is sensitive to all a-particles

reaching its surface.
Disk shaped Pershore Mouldings CR-39 (500 mm An a-particle i with an initial energy Eai emitted
thickness) and Kodak LR-115 type II (12 mm cellulose from a nucleus localized on point M inside the ma-
nitrate on 100 mm polyester base) SSNTD lms of 4 terial sample studied (Fig. 2) has a range R*i
cm diameter have been separately placed on a homo-
R*i x RD , 1
geneous material sample in a hermetically sealed
cylindrical plastic container (Fig. 1) for one month and where x (xR Ri, Ri is the range of the a-particle inside
a half. During this time a-particles emitted by the the material sample) is the distance between the emis-
uranium and thorium series bombarded the SSNTD sion point and the surface of the SSNTD (Fig. 2) and
lms. After the irradiation, the bombarded lms were RD is the range of the a-particle in the SSNTD. The a-
developed in a NaOH solution (2.5 N at 608C during particle residual energy E Res
ai (Fig. 2) which can be de-
120 min for LR-115 lms and 6.25 N at 708C during 7 rived from Ri x is determined using the energy-range
h for the CR-39 sheets). After this chemical treatment relation for the considered samples (Fig. 3). The E Res
ai
the track densities registered on the CR-39 and LR- residual energy corresponds to the RD range inside the
115 SSNTD were determined by means of an ordinary CR-39 SSNTD (Fig. 4) and RD 0 range inside the LR-
115 SSNTD (Fig. 5).
microscope. In the case of radioactive equilibrium in
The critical angles of etching of the CR-39 (yc) and
the material samples studied, eight a-particles per 238 U
LR-115 (yc 0 ) SSNTD (determined from the normal to
disintegration and six a-particles (from seven daughter
the detector surface) are respectively given by Somogyi
nuclides) per 232 Th are emitted. We assume a secular et al. (1984) and Jonsson (1981)
equilibrium between radon (222 Rn) and its radium 226
(226 Ra) parent. For our experimental etching con- 1
cos yc 2
ditions, the residual thickness of the LR-115 type II 11:6R0:464
D
SSNTD is 5 mm which corresponds to the lower and
(Emin = 1.6 MeV) and upper (Emax = 4.70 MeV)
energy limits for registration of tracks of alpha par- 1
cos yc 0 , 3
ticles in LR-115 type II lms. All a-particles emitted 1 e0:27RD 0 3
by the uranium and thorium series that reach the LR- where the ranges RD and RD 0 are in mm.
115 SSNTD with a residual energy situated between The average value of the critical angle of etching is
1.6 MeV and 4.7 MeV are registered as bright track- given by:

Fig. 1. Arrangement of the solid state nuclear track detectors on a material sample in a well closed cylindric plastic container of 2
cm radius and 1 cm depth.
 M.A. Misdaq et al. / Applied Radiation and Isotopes 51 (1999) 209215 211

Fig. 2. Trajectory of an a-particle inside the material sample (MI = x) and SSNTD (IF = RD). Eai is the initial energy of the a-par-
ticle and E Res
ai its residual energy on the point I.
Ea
1 i
The last relation is
hyc 0 i yci E Res Res
ai dE ai 4
Eai 0
dNi li $i dVte , 7
for the CR-39 SSNTD and
where $ i is the number of a-emitters of index i per
unit volume.
1 Emax 0 Res
hyc 0 i yc E ai dE Res
ai 5 Let dMi represent the number of a-particles of
DE Emin
energy Eai emitted (in the volume dV) during the ex-
for the LR-115 SSNTD where DE = Emax Emin, posure time te which reach the SSNTD lm
yci E Res
ai and yc 0 E Res
ai represent the analytical dO
0
equations of the critical angles yci and yc as a function dMi li $ i dV te , 8
4p
of the a-particle residual energy (E Res
ai ).
Let us consider an elementary cylinder of volume where dO = 2p siny dy is the elementary solid angle.
dV, surface base dS and depth dh inside the material According to Fig. 1, we have
sample (Fig. 1). dS dS 0 cos y, 9
Let dNi represent the number of a-particles i with
0
an energy Eai emitted from the radioactive nuclei (in where dS is an elementary surface of the SSNTD lm.
the volume dV) during the exposure time te: Eq. (8) could be rewritten:
dNi li dni te , 6 cosy siny
dMi li $ i te dS 0 dh dy 10
2
where dni is the number of a-emitters of index i in the
The numbers of a-particles i with an energy Eai
volume dV and li the decay constant.
emitted in the volume dV which reach and are regis-

Fig. 3. Alpha particle rangeenergy relation for a granite ma- Fig. 4. Alpha particle rangeenergy relation for the CR-39
terial sample. solid state nuclear track detector.
212 M.A. Misdaq et al. / Applied Radiation and Isotopes 51 (1999) 209215

tered on the CR-39 and LR-115 SSNTD per unit area 3. Results and discussion
and unit exposure time are respectively given by:
The residual energy E Res ai of the a-particles emitted
sin2 yci by the uranium and thorium families inside dierent
rCR
i li $ i Ri 11
4 material samples have been calculated by using the
and corresponding energy-range relations (an example is
given in Fig. 3). The critical angles of the CR-39 (yc)
sin2 yci 0 and LR-115 (yc 0 ) SSNTD for detecting a-particles of
rLR
i li $i DR, 12
4 the uranium and thorium series have been evaluated
where DR = Rmax Rmin. Rmin and Rmax are the a-par- by using the corresponding alpha particle rangeenergy
ticle ranges in the sample which correspond to the relations shown in Figs. 4 and 5 and Eqs. (2) and (3).
lower (Emin = 1.6 MeV) and upper (Emax = 4.7 MeV) Data obtained for the critical angle yc of the CR-39
ends of the energy window (DE = Emax Emin). SSNTD are shown in Table 1. We notice that yc
Assuming a secular equilibrium between uranium, depends on the initial energy of the emitted a-particles:
thorium and their corresponding daughters, the global for a given material, yc decreases when the a-particles
track density rates (tracks cm 2 s 1 ) due to the a- initial energy increases. We also notice that the critical
particles of the uranium and thorium series, registered angle yc depends on the residual energy of the a-par-
on the CR-39 (rCR LR
G ) and LR-115 (rG ) SSNTD are re-
ticles (E Res
ai ): for a given material and a given a-particle
spectively given by initial energy (Eai ) yc increases when the residual
energy (E Resai ) decreases (Fig. 6). The relative uncer-
X8 tainty of the yc critical angle determination is about
rCR
G 0:25dS Au Bq=gCU sinhyci i2 ki Ri 1%. Results obtained for the a-particles emitted by the
i1
nuclei of the uranium and thorium series inside a clay
X
7 material sample are shown in Fig. 6. For the uranium
Ath Bq=gCTh sinhyci i2 ki Ri 13 and thorium contents determination in various ma-
i1 terials, the critical angle yc should be evaluated for
and each a-particle initial energy, Eai , and an average value
should be determined for the corresponding residual
0 2
rLR
G 0:25ds
DR
sinhyc i 8
Au Bq=g
CU energies (E Res
ai ). Results obtained for the average value
of yc (Eq. (4) and Fig. 6) (hyci) for a-particles emitted
6
Ath Bq=g
CTh 14 by the uranium and thorium series are shown in
where ds is the density of the material sample (g cm 3), Table 2. We notice that hyci does not depend on the
Au (Bq/g) is the specic activity of the sample for a nature of the material sample: an average
238
U content of 1 ppm (10 6 g/g), Ath (Bq/g) is the hyci = 73.98 2 0.58 has been found for a-particles
specic activity for 1 ppm of 232 Th, Ri is the range of emitted by the uranium and thorium series inside the
an a-particle of initial energy Eai and index i in the materials studied. This result is in good agreement
material sample, hyci i is the average value of yci in the with data given in literature: an average yc = 758
[Eai 0 MeV] residual energy range, hyc 0 i is the average (determined from the normal to the detector surface)
value of yc 0 in the [1.64.70 MeV] energy window. was found to be suitable for a-particles emitted by the
Combining Eqs. (13) and (14), we obtain the follow- uranium and thorium families inside various geological
ing relationship be**tween track density rates and samples (Hafez and Naim, 1992).
thorium to uranium ratios:

X
8 X
7
Au Bq=g sinhyci i2 ki Ri Ath Bq=gCTh=CU sinhyci i2 ki Ri
rCR
G i1 i1
: 15
rLR
G DR
sinhyc 0 i2 8Au Bq=g 6Ath Bq=gCTh=CU

Measuring rCR LR
G and rG track density rates and calcu- Variation of yc 0 as a function of the initial and re-
0
lating hyci i and hyc i one can evaluate the C(Th)/C(U) sidual energies of the a-particles emitted by uranium
ratio and consequently the thorium C(Th) (in ppm) 238, thorium 232 and their corresponding daughters
and C(U) (in ppm) contents in a given material inside a clay sample are shown in Fig. 7. We notice
sample. that inside the DE [1.64.7 MeV] energy window yc 0
 M.A. Misdaq et al. / Applied Radiation and Isotopes 51 (1999) 209215 213

Fig. 5. Alpha particle rangeenergy relation for the LR-115

type II solid state nuclear track detector, obtained using a
TRIM programme (Biersack and Ziegler, 1992).
Fig. 6. Variation of the CR-39 critical angle (yc) versus the re-
sidual energy of the a-particles emitted by the 212 Po nuclei
depends strongly on the residual energy of the a-par- (Eai = 8.78 MeV) inside a clay sample.
ticles emitted by the uranium and thorium families
inside the considered material samples.
Data obtained for the average value of the critical
The relative uncertainty of the hyc 0 i critical angle deter-
angle yc 0 , hyc 0 i (Eq. (5) and Fig. 7), for a-particles
mination is about 4%.
emitted inside the considered materials which reach the
We notice that the critical angle of the CR-39
LR-115 detector with residual energies belonging to
SSNTD is higher than that of the LR-115 type II one
the energy window (DE) (Table 3) are in good agree-
ment with results found by Hafez and Naim (1992) for detecting a-particles emitted by the uranium and
and Jonsson (1981). Indeed, these authors obtained an thorium series inside the materials studied in agree-
average value of 508 (determined from the normal to ment with literature (Somogyi, 1980; Hafez and Naim,
the detector surface) for the critical angle of the LR- 1992). The CR-39 registering eciency is greater than
115 type II SSNTD for a residual thickness of 5 mm. that of the LR-115 SSNTD.

Table 1
Data obtained for the CR-39 critical angle for detecting full
energy a-particles emitted by the uranium and thorium series
inside a clay sample
Table 2
Data obtained for the average value of the CR-39 critical
angle (hyci) for detecting a-particles, of various initial ener-
gies, emitted by the uranium and thorium series inside a clay
sample

Nuclides Alpha The critical Nuclides Alpha Average

particle angle of the particle value of the
initial CR-39 SSNTD initial CR-39 critical
energy (8) energy angle (hyci)
(MeV) (MeV) (8)

232 232
Th 4.01 68.920.6 Th 4.01 77.220.4
238 238
U 4.19 68.320.6 U 4.19 76.820.4
230 230
Th 4.62 66.920.7 Th 4.62 75.920.5
234 234
U 4.77 66.420.7 U 4.77 75.620.5
226 226
Ra 4.78 66.320.7 Ra 4.78 75.620.5
210 210
Po 5.30 64.620.7 Po 5.30 74.620.5
228 228
Th 5.42 64.220.7 Th 5.42 74.420.5
222 222
Rn 5.49 63.920.8 Rn 5.49 74.320.5
224 224
Ra 5.71 63.320.8 Ra 5.71 73.820.5
218 218
Po 6.00 62.320.8 Po 6.00 73.320.5
212 212
Bi 6.05 62.220.8 Bi 6.05 73.220.5
220 220
Rn 6.29 61.420.8 Rn 6.29 72.820.6
216 216
Po 6.78 59.920.9 Po 6.78 71.920.6
214 214
Po 7.68 5721 Po 7.68 70.320.7
212 212
Po 8.78 5421 Po 8.78 68.520.7
214 M.A. Misdaq et al. / Applied Radiation and Isotopes 51 (1999) 209215

Table 3
Data obtained for the average value of the LR-115 critical angle (hyc 0 i) for detecting a-particles emitted by the uranium and thor-
ium series inside dierent material samples, which reach the SSNTD with residual energies belonging to the energy window

Material Clay Cement Water Granite Phosphate Plaster

hyc 0 i 462 2 462 2 46 22 462 2 46 22 462 2

Table 4
Data obtained for uranium (C(U)} and thorium (C(Th)) contents in dierent geological material samples

Sample rCR
G (10
+4
) rLR
G (10
+4
) This method Isotope dilution mass
(tracks cm 2 s 1) (tracks cm 2 s 1) spectrometry

C(U) C(Th) C(U) C(Th)

(ppm) (ppm) (ppm) (ppm)

YAR 62 (basalt) 3.7 20.1 1.3020.04 2.5 20.1 0.38 20.02 2.47 20.03 0.40 20.01
YAR 82 (basalt) 5.4 20.1 1.7920.04 1.57 20.04 8.0 20.2 1.53 20.02 8.1 20.1
B3 (basalt) 4.2 20.1 1.4120.04 2.14 20.07 3.2 20.2 2.23 20.04 3.18 20.04
NA2 (basalt) 3.0 20.1 1.0020.04 1.14 20.06 3.5 20.2 1.20 20.02 3.65 20.04
YJ23 (microdiorites) 7.7 20.2 2.5220.06 3.8 20.1 6.5 20.4 3.77 20.04 6.5 20.1
YJ25 (microdiorites) 6.4 20.2 2.1920.05 2.7 20.1 7.1 20.4 2.67 20.03 6.9 20.2
DZ1 (dolerite) 1.9 20.1 0.6620.04 1.10 20.07 0.90 20.06 1.15 20.02 0.94 20.01
DZ2 (dolerite) 3.0 20.1 1.0320.03 1.60 20.06 2.0 20.1 1.55 20.02 2.05 20.02

The C(Th)/C(U) ratio as well as thorium and
uranium contents in basalt (B3, Yar 62 and Yar 82)
and dolerite (DZ1, DZ2 and NA2) samples collected
from the permotriasic Argana basin (south of
Marrakech) as well as in microdiorite (YJ23 and YJ25)
samples collected from the `permian' microdiorite of
the Jbilet area (north of Marrakech) have been deter-
mined (Eqs. (13)(15)). Data obtained by this method
are in good agreement with those obtained by using
isotope dilution mass spectrometry (Table 4). The rela-
tive uncertainty of the uranium and thorium contents
determination is about 7%.
4. Conclusion
It has been shown by this study that the critical
angles of etching of the CR-39 and LR-115 type II
solid state nuclear track detectors (SSNTD) for detect-
ing a-particles emitted by the nuclei of the uranium
and thorium series inside dierent material samples
depend on the initial and residual (at the entrance of
the SSNTD) energies of the considered a-particles. A
new method based on exploiting data obtained for the
CR-39 and LR-115 SSNTD mean critical angles and
measuring the track density rates registered on these
detectors for evaluating the uranium and thorium con-
tents in various geological samples has been developed.
Results obtained are in good agreement with data
obtained by using isotope dilution mass spectrometry.
This method has the advantage of being simple, mod-
erately accurate, inexpensive and nondestructive.

Fig. 7. Variation of the LR-115 critical angle (yc 0 ) versus the
residual energy of the a-particles emitted by the uranium and
thorium series inside a clay sample. The residual thickness of
the LR-115 SSNTD is 5 mm.
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