Radiation Meuuremen~

PERGAMON Radiation Measurements31 (1999)437--442

OPTIMIZATION OF CR-39 FOR FAST NEUTRON

DOSIMETRY APPLICATIONS

E. VILELA*'**, E. FANTUZZI**, G. GIACOMELLI*, M. GIORGINI*,

B. MORELLI**, L. PATRIZII*, P. SERRA* AND V. TOGO*
INFN Viale Berti-Pichat, 6/2 1-40127 Bologna, Italy
**ENEA Via dei Colli, 16 1-40136 Bologna, Italy
ABSTRACT
We present the results of an experimental work aimed at improving the performances of
the CR-39 ® (Registered Trademark of PPG Industries Inc.) nuclear track detector for
neutron dosimetry applications. The work was done in collaboration with the Intercast
Europe S.p.A., producer of CR-39 for commercial and scientific applications. We compare
the CR-39 made with different additives concentrations and different polymerization
~rocesses. We evaluate the response of the CR-39 to fast neutrons from three sources:
~Am-Be, 2S2Cfand 238pu-Li. Particular attention was paid to background fluctuations
that limit the lower detectable dose.

KEYWORDS
CR-39; fast neutron dosimetry; additive; dopant; polymerization processes.

INTRODUCTION
Since few years the Bologna section o f the INFN (Italian National Institute o f Nuclear Physics)
together with the Intercast Europe S.p.A. have worked together to develop a better and more
appropriate CR-39 material for scientific applications. This material is nowadays in use for the
detection of different particles in fundamental physics in Italy and worldwide (Giacomelli and Popa,
1997; Derkaoui et al, 1998).

Two years ago the Dosimetric Service of the ENEA (Italian National Agency for New Technologies,
Energy and the Environment) has initiated a series of tests of this CR-39 for neutron dosimetry
applications. It was noticed that this material shows a satisfactory response to be employed in this
field (Morelli et al., 1998a). However this study demonstrated that it would be interesting to produce
a CR-39 specifically optimized for the requirements of a fast neutron dosimetric service.

Based on the ENEA Dosimetric Service experience the following points have been checked: a) the
possibility of obtaining a more transparent material, even after a prolonged etching; b) no significant
differences in response between both sides of a foil; c) a more stable polymer that could be stored for
long periods without losing its initial properties; d) to have a material with a higher contrast between
the track and the CR-39 surface (it could be obtained by adding a colorant to the original composition).

With these aims in mind, we checked the response to fast neutrons o f CR-39 foils different
compositions for which we varied the DOP (dioctyl phthalate) concentrations; we added the

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438 E. Vilela et al. / Radiation Measurements 31 (1999) 437-442

antioxidant Naugard 445 (N445) (Doke et al., 1988) and introduced a colorant. Another point to verify
was the material response when the polymerization process was modified.

To evaluate the CR-39's response we considered the following parameters: the materials sensitivities,
the background track density and reproducibility, and the lower detectable dose. The variability of
such parameters as function of the neutron incident energy was also determined.

The general characteristics and compositions of the investigated types of CR-39 are presented in
Table 1.

Table 1. General characteristics of the used CR-39's.

Material Date of DOP (%) N445 (%) Thickness Polymerization Colorant
ID production (gm)
type (%)
A 1/30/98 0.4 0.01 1500 Vertical/water 0
B 1/30/98 0.4 0.01 1500 Horizontal/air 0
C 1/30/98 0.2 0.01 1500 Vertical/water 0
D 1/30/98 0.2 0.01 1500 Horizontal/air 0
E 2/6/98 0 0 1500 Vertical/water 0
F 2/6/98 0 0 1500 Horizontal/air 0
G 2/6/98 0.2 0 1500 Vertical/water 0
H 2/6/98 0.2 0 1500 Horizontal/air 0
I 2/6/98 0 0 700 Vertical/water 0
L 2/11/98 0 0 700 Horizontal/air 0
M 2/11/98 0 0.01 700 Vertical/water 0.12
N 2/11/98 0 0.01 700 Horizontal/air 0.12

EXPERIMENTAL

Irradiations

Irradiations have been carried out at the Radiation Protection Institute of ENEA. A set of nine
dosemeters of each material was exposed to a fast neutron dose equivalent of 2 mSv (ICRP74, 1997)
from the 24tAm-Be, 252Cf and 23SPu-Li sources, with mean energies of 4.3 MeV, 2.1 MeV and 0.6
MeV, respectively (Griffith et al., 1990).

Processing
Before irradiations the CR-39 sheets were lasercut in pieces of dimensions of 25 x 36 mm 2. Each
piece was marked so that it was possible to identify the front and back sides. For horizontal
polymerization the back side was defined as the upper side of the foil. For the vertical one the back
side was taken as the face farther away from the neutron source. This resulted in a self radiator effect
from the thickness of the detector. This effect was also considered for irradiation of the detector with
horizontal polymerization. The twelve materials were divided in three sets each composed of nine
irradiated and 27 non irradiated detectors for background evaluation.
 E. l~lela et aL / Radiation Measurements 31 (1999) 437-442 439

The three sets of detectors were etched employing the same procedure of the Dosimetric Service, that
consists in a 30 min. pre-etching in a mixture of 60% ethyl alcohol and 40% 6.25 N KOH solution at
70°C followed by a 12 h etching in 6.25 N KOH solution at 70°C (Morelli etal., 1998b).

Detectors were read out using a system composed of an optical microscope connected to an image
analyzer. The counting of the tracks is performed by an on-line computer. In this system, light is
channeled through the detector so that just a surface of the detector is viewed by the system at a time.
In order to evaluate the influence o f the polymerization process both sides o f each detector were
analyzed. A total area of 1.17 cm 2 for each surface was scanned. To reduce the background due to
material surface defects, optimization of contrast between track image and material surface was made.

RESULTS

Polymerization processes

Materials from two different processes of CR-39 polymerization were analyzed. The first one was
carried out with CR-39 molds in horizontal position and surrounded by air, the second one with molds
in the vertical position surrounded by water. This study aimed to obtain a material with no significant
difference in response between the two faces.

Figures 1 and 2 show the responses for the t w o different polymerization methods and for different
energies. We observe that the differences on the polymerization process practically do not alter the
sensitivity of the materials when considering the same face of the materials (in the figures are only
shown the responses for the back sides).

When considering the two different faces (front and back) the energy dependence of the response is
significant. It was also possible to verify that the background level in the detectors manufactured with
the vertical polymerization was larger than for horizontal polymerization. This is due to a stronger
effect o f sedimentation during the vertical polymerization process; it results in a less uniform
background response along the vertical direction of the foils (Figs. 3 and 4).

900- 900
800- • 241Am-Be 800- • 241Am-Be
700- [ ] 252Cf A 700- [ ] 252Cf
• 238Pu-Li

soo- ~ soo-
40o- ~ 400-
¢ 300-
~ 200-
too-
O-
B D F H
MaterialID
L N
~ 300-
[E 200-
Ioo-
O
bh,bLkL
A C E G
MaterialID
I M

Fig. 1. Response of the different Fig. 2. Response of the different

CR-39 polymerized horizontally in CR-39 polymerized vertically in
air. The response as function of the water.
neutron incident energies is also
reported.
440 E. lqlela et al. / Radiation Measurements 31 (1999) 437-442

8OO
• 241Am-Be 30O
[] 2S2Cf
25O
i • Back
• 238Pu-Li [] Front
200-
E
150-

~ 100-
®
R ~ N 1] I1-

F back F front
"I,| i.LJlJdj,l||,d|[!LJj!llJ
Material ID Det~or ID

Fig. 3. Comparison of the back and Fig. 4. Comparison of the back and
front faces responses of the CR-39 front faces of the detectors
type F. background for CR-39 type F.

0.5

0.4
• 241Am-Be >
(O
iit • 241 Am-Be I

E [] 252Cf g
• 238Pu-Li
0.3
J~
o

B D F H L N A C E G I M
Material ID Material ID

Fig. 5. Lower detectable dose (mSv) Fig. 6. Lower detectable dose (mSv)
for each investigated material. for investigated material. Vertical
Horizontal polymerization in air. polymerization in water.

The larger background and lower reproducibility of the vertical polymerization is reflected on the
increase of the lower detectable dose (LDD) (see figures 5 and 6). The LDD values were calculated as
3Gbs/S where trbg is the standard deviation o f the background and S is the material sensitivity in units
tracks cm"2 mSv"/ (Schraube et ai., 1995).

DOP concentration
In order to vary the material transparency we introduced an increasing DOP percentage in the CR-39
composition. The decrease of the material sensitivity versus increasing DOP concentration is shown in
Fig.7. From figures 5 and 6 we observe that the values of the lower detectable dose increase by a factor
of 59% when adding 0.2% in mass o f DOP (materials H and F); the effect of DOP combined with
N445 on the polymer sensitivity was significant (materials D and F).

The background track density reproducibility was obtained for all three materials containing DOP (B,
D and H) of the order of 40%, this represents an improvement when compared with the pure material
 E. Vilela et al. / Radiation Measurements 31 (1999) 437-442 441

(F) with 45% of reproducibility. The increase in the lower detectable dose was attributed to the loss in
the sensitivity arising from the additives.

700
¢ 241Am-Be
> 600
09 zx 252Cf
E
500 n 238Pu-Li
E
400

= 300
o
I

rr 200

I00
0'.0 0'.1 0'.2 0'.3 0'.4 0.5
DOP concentration (%)

Fig.7. Dependence of the response as function of the DOP concentration.

N445 antioxidant
The Naugard 445 was added in order to increase the stability of the material stored for long periods.
The antioxidant may possibily increase the sensitivity and reduce the average background, resulting in
better values o f the lower detectable dose ( histograms A and C of Fig. 6, and B and H of Fig. 5, in
histograms M and N colorant is also present ), However a more detailed investigation is necessary.

Colorants
With the read out system used at the ENEA Dosimetric Service the addition of a colorant to the CR-39
would facilitate the analysis of the dosemeters because of the increasing of the contrast between track
areas and detector surface. Therefore a small quantity of red colorant (0.12%, in mass) was added. This
colorant is commonly used in CR-39 for commercial applications.

The addition of such a colorant had only a small influence on the CR-39 sensitivity, but it decreased
the reproducibility of the response. It is important to note that the contrast of the material was
increased. A summary o f the influence of the colorant on the CR-39 response, background,
reproducibility and LDD is given in table 2.

Table 2: Comparison of the behaviour of the different materials as function of the presence of a
colorant.

Materials Response (241Am-Be) Background cbg (%) LDD

ID (tr cm "2 mSv "l) (tr cm "2) (pSv)

M 478 + 9 40 + 5 68 168
N 487 + 16 31 + 3 53 102
L 591 + 25 68 + 3 25 78
442 E. Vilelaet al. / RadiationMeasurements31 (1999)437-442

CONCLUSIONS
In this paper are presented preliminary results on the development of a better CR-39 nuclear track
detector for applications in fast neutron dosimetry.

The addition of DOP is not recommended, even when employed in small quantities.

The recommended polymerization process is that in air in the horizontal position; even if this process
brings differences between the two faces, it seems to yield a material which is more stable and with a
more reproducible background.

The used antioxidant seems not to affect in a sensitive way the response.

The colorant reduces the background, but it also reduces the sensitivity resulting in an increase of the
LDD.

Work is in progress to study the response to energies lower than 500 keV.

Acknowledgment -- The authors thank ENEA, 1NFN and 1NTERCAST Europe S.p.A. for providing fellowships
and grants, especially for non-Italian citizens.

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