Radiation Protection Dosimetry (2006), Vol. 120, No. 1–4, pp.

457–460
doi:10.1093/rpd/nci675 Advance Access published on May 30, 2006

NEUTRON SPECTROMETRY USING CR-39 TRACK ETCH

DETECTORS
Gary W. Phillips1,, Jerrette E. Spann1,3, James S. Bogard2, Tuan VoDinh2, Dimitris Emfietzoglou1,4,
Robert T. Devine5 and Marko Moscovitch1
1
Georgetown University, Radiation Medicine Department, 3970 Reservoir Road NW, Research
Building Room E202A, Washington, DC 20057-1482, USA
2
Oak Ridge National Laboratory, P.O. Box 2008, Oak Ridge, TN 37831-6480, USA
3
Washington Hospital Center, Radiation Safety, 110 Irving Street NW, Washington, DC
20010-2975, USA
4
University of Ioannina Medical School, Medical Physics Department, Ioannina 451 10, Greece

Downloaded from http://rpd.oxfordjournals.org/ at University of Notre Dame on August 23, 2014

5
Los Alamos National Laboratory, MS G761, P.O. Box 1663, Los Alamos, NM 87545, USA

Track-size distributions were measured for chemically etched CR-39 foils exposed to monoenergetic neutrons with energies
ranging from 0.144 to 19 MeV and to various broad-spectrum neutron sources including spontaneous fission neutrons from
238
Pu. These tracks are due to energetic charged particles resulting from interactions of the neutrons with the CR-39. The
tracks are visible with an optical microscope after chemical etching and vary in size and configuration depending on the
particle, energy and angle of incidence. The foils were analysed using an automatic analysis system that scans the foils,
identifies valid tracks and records the track-size parameters. The track-size distributions vary with neutron energy for the
monoenergetic sources and with the hardness of the broad-spectrum sources. The distribution from the 238Pu fission source is
readily distinguishable from the other sources measured and from distributions owing to the background.

INTRODUCTION 0.144 to 19.0 MeV. The foils were arranged on the

Neutron elastic interactions with CR-39 plastic
(poly-allyl diglycol carbonate, formula C12H18O7)
leave latent recoil charged particle tracks that can
be brought out by chemical or electrochemical etch-
ing. Above a threshold of 7.9 MeV, inelastic alpha
particle breakup of 12C is also possible with the
energy lost by the neutron partitioned among the
three alpha particles(1). The size and characteristics
of the tracks depend upon the charged particle mass,
energy and direction. Energy dependence has been
reported previously of the distribution of track sizes
for monoenergetic neutrons(2,3) and for broad-
spectrum neutrons(4,5). Fleischer et al. have investig-
ated the dependence of the track density with energy
and fluence(6) and with direction(7). In the present
work, track-size distributions were measured for an
expanded range of energies and sources and distri-
butions were obtained which agree in general but
differ in detail where the measurements overlap
with the previous reports.
MONOENERGETIC NEUTRON EXPOSURES
CR-39 foils 1.6 mm thick, obtained from Track
Analysis Systems Limited (TASL), Bristol, UK,
were exposed to monoenergetic neutrons at
Physikalisch-Technische Bundesanstalt, Braunsch-
weig, Germany with neutron energies ranging from

Corresponding author: phillipg@georgetown.edu
faces of a truncated pyramid of polystyrene. Thus,
there was significant exposure of the foils to scat-
tered neutrons from the polystyrene in addition to
direct neutrons from the beam. For each neutron
energy, four foils were exposed at an angle of 0
and six at an angle of 60 normal to the beam.
After exposure, the foils were etched according to
the method of Harvey and Weeks(8). A pre-etch was
done for 1 h in 60% ethanol, 40% 6.25 M NaOH mix
at 70 C, which uniformly removed 60 mm from
each face. This was followed by a 6 h etch in 6.25 M
NaOH solution at 70 C, which preferentially etches
along the tracks. The neutron mean free paths are
long compared with the foil thicknesses so that the
recoil particle tracks begin uniformly throughout
the foil. During the 6 h etching time some tracks
may be etched away but others will be revealed.
The pre-etch reduces the surface bias, which results
in fewer tracks near the original front surface since
no tracks originate beyond the surface. After etch-
ing, the tracks were observed under a microscope
and were found to have images ranging from 2 to
40 mm in size. Tracks that enter perpendicular to the
face produce a circular image while those that enter
at an angle produce an elliptical or teardrop-shaped
image.
The etched foils were analysed using an automatic
system by TASL which scans each foil frame by
frame, transfers the microscope images to a com-
puter and analyses the images for tracks which
satisfy certain preset parameters. The computer pro-
gram saves the x, y position, long and minor axes for

Published by Oxford University Press (2006)

 G.W. PHILLIPS ET AL.

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Figure 1. CR-39 efficiencies as a function of neutron
energy averaged over foils with their faces oriented at 60
and at 0 normal to the beam. The mean 60 to 0
efficiency ratio over all energies is 0.80  0.04. The error
bars indicate the standard deviations in the measurements
for foils of the same energy and orientation.

each track. Figure 1 shows the efficiencies in tracks

per neutron (tracks per unit area divided by neutron
fluence) averaged separately at each energy over the
foils exposed at 0 and at 60 to the beam. The
efficiencies found here are several times larger than
those reported earlier by Fleischer et al.(6), who used
a shorter etching time of 3.75 h at 60 C and no pre-
etch. Shorter etching leaves fewer features but results
in more clearly defined tracks. The standard devi-
ations for foils of the same energy and orientation
are indicated by the error bars in Figure 1 and aver-
age 21%, which is well beyond the statistical uncer-
tainties. There is a trend of increasing efficiency with
neutron energy up to 1 MeV, above which it is
approximately flat. The average efficiency ratio at
60 to 0 is about 0.8, compared with a solid angle
ratio of 0.5 as seen from the beam direction. Thus,
for dosimetry purposes the energy and angular
dependencies are moderate but not negligible. In
comparison, Fleischer and Paretzke(7) saw large
differences for foils at 0 and 90 to the beam
but these were exposed without the polystyrene scat-
terer used here.
Figure 2 shows the distributions of the number of
tracks versus the long-axis track size, plotted for
each neutron energy. There were no significant
differences in the track-size distributions at 0 and
60 so these were combined in the figure. The distri-
butions of the ratios of the minor axis to the long
axis were also examined to look for directionality
between the 0 and 60 foils. There was a slight
difference at 0.144 MeV but no significant differ-
ences for the higher energies.
The track size depends both on the linear energy
transfer (LET) along the track and on the range, as
458
Figure 2. CR-39 track-size distributions for monoenergetic
neutrons with energies ranging from 0.144 to 1.2 MeV
(upper panel), from 1.2 to 8.0 MeV (middle panel) and
from 8.0 to 19.0 MeV (lower panel).
well as on the etching parameters. At low energies
only the protons will have sufficient range to leave a
visible track. Figure 2 (upper panel) shows the track-
size distributions for neutron energies between 0.144
and 1.2 MeV. These distributions are clearly distin-
guishable. As the neutron energy increases, there is a
broadening of the proton recoil peak at 10 mm. At
1.2 MeV neutron energy a second peak is visible at
25 mm, probably owing to recoil carbon and
oxygen ions(4).
Figure 2 (middle panel) shows the distributions for
neutron energies between 1.2 and 8.0 MeV. These
distributions are roughly similar although they differ
in detail. Figure 2 (lower panel) shows the distribu-
tions for neutron energies between 8.0 and 19.0
MeV. These are again clearly distinguishable, with
two notable features: (1) the proton recoil peak at
10 mm declines with increasing neutron energy and
decreasing recoil proton LET and (2) in the distribu-
tions for 14.8 and 19.0 MeV neutrons there is a
significant peak at 30–35 mm likely due to three
alpha particle reactions. Thus in the range of
 CR-39 NEUTRON SPECTROMETRY
Figure 3. IAEA reference neutron source spectra.
Figure 4. CR-39 track-size distributions for broad-
spectrum fission neutron sources 252Cf, D2O-moderated
252
Cf, 238PuO and a transit foil (upper panel) and for
alpha-beryllium neutron sources 239PuBe, 238PuBe and
241
AmBe (lower panel).
neutron energies <1.2 MeV and >8 MeV the track-
size distributions are quite distinct, while at the inter-
mediate neutron energies the distributions are sim-
ilar and less readily distinguishable.
BROAD-SPECTRUM NEUTRON EXPOSURES
CR-39 foils were exposed to the following broad-
spectrum neutron sources to determine if their
459
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Figure 5. Ratios of CR-39 track-size distributions between
15 and 20 mm to those between 20 and 25 mm (upper panel)
and of distributions between 15 and 20 mm to those
between 25 and 30 mm (lower panel). The error bars indic-
ate the standard errors in the data.
track-size distributions were distinguishable: 238PuO,
252
Cf, D2O-moderated 252Cf, 238PuBe, 239PuBe and
241
AmBe. The International Atomic Energy Agency
has tabulated neutron energy spectra for these
sources(9) although the IAEA tables do not specify
isotopic composition except for 252Cf. These spectra
are shown in Figure 3. In order of increasing hard-
ness, the PuO spectrum has a relatively sharp peak at
1 MeV. The unmoderated 252Cf spectrum has a
single broad peak at 2 MeV, whereas the D2O-
moderated 252Cf spectrum is multi-modal, with
peaks at 2, 0.5 and 0.01 MeV. Finally, the PuBe
and AmBe spectra have broad peaks extending from
3 to 6 MeV. Unlike the previous monoenergetic
exposures, the CR-39 foils were exposed to these
sources in a lightweight holder that contributed few
backscattered neutrons. These foils were then etched
in 6.25 M NaOH solution at 98 C for 90 min with no
pre-etch. Figure 4 (upper panel) shows the long-axis
track-size distributions for the three spontaneous
fission sources: 252Cf, D2O-moderated 252Cf,
238
PuO and a transit foil that was unexposed.
 G.W. PHILLIPS ET AL.
238
The distribution for the PuO source drops off
rapidly between 20 and 25 mm while the distribution
for the two 252Cf sources extends out to 25 mm and
beyond. Figure 4 (lower panel) shows the distribu-
tions for the three alpha-beryllium sources: 239PuBe,
238
PuBe and 241AmBe. The distributions for these
sources all extend out beyond 25 mm.
Figure 5 compares these distributions by showing
the ratios of the number of tracks with their long
axes between 15 and 20 mm to those with axes
between 20 and 25 mm (upper panel) and of the
number of tracks between 15 and 20 mm to those
with axes between 25 and 30 mm (lower panel). Both
ratios are significantly larger for 238PuO than for
the other sources while in the 25–30 mm range the
ratios for the D2O-moderated 252Cf and the
241
AmBe sources are significantly larger than
those for the unmoderated 252Cf source and the
two PuBe sources. Clearly the long-axis distributions
can be used to distinguish the 238PuO fission source
from the harder spectrum sources and can possibly
be used to distinguish between some of the other
sources.
SUMMARY AND CONCLUSIONS
The data for the monoenergetic neutron sources
show that the CR-39 track-size distributions can be
used to distinguish sources in the energy range of
0.144–1.2 MeV and the range of 8.0–19.0 MeV. Dis-
tributions for sources in the range of 1.2–8.0 MeV
are similar and would be more difficult to distin-
guish. The distributions for the broad-spectrum
neutron sources show that 238PuO source, which
has a softer neutron energy spectrum, can be readily
distinguished from the unmoderated 252Cf, D2O-
moderated 252Cf, 238PuBe, 239PuBe and 241AmBe
sources, all of which have harder neutron spectra.
460
ACKNOWLEDGEMENTS
This work was supported in part by the National
Nuclear Security Agency, US Department of Energy
and by the Defense Threat Reduction Agency, US
Department of Defense.
REFERENCES
1. Fleischer, R. L., Price, P. B. and Walker, R. M. Solid
state track detectors: applications to nuclear science and
geophysics. Ann. Rev. Nucl. Sci. 15, 1–28 (1965).
Downloaded from http://rpd.oxfordjournals.org/ at University of Notre Dame on August 23, 2014
2. Hankins, D. E. and Westermark, J. Preliminary study
on the use of the track size distributions on electrochem-
ical etched CR-39 foils to infer neutron spectra. Radiat.
Prot. Dosim. 20(1/2), 109–112 (1987).
3. D’Errico, F., Weiss, M., Luszik-Bhadra, M., Matzke, M.,
Bernardi, L. and Cecchi, A. A CR-39 track image ana-
lyzer for neutron spectrometry. Radiat. Meas. 28(1–6),
823–830 (1997).
4. Jakes, J. and Schraube, H. Etched track size distribu-
tions induced by broad neutron spectra in PADC. Radiat.
Prot. Dosim. 70(1–4) 133–138 (1997).
5. Anderson, M. E. and Neff, R. A. Neutron energy spec-
tra of different size 239PU-Be(n, a) sources. Nucl.
Instrum. Meth. 99, 231–235 (1972).
6. Fleischer, R. L. et al. Personnel neutron dosimetry using
particle tracks in solids: a comparison. Health Phys. 47,
525–531 (1984).
7. Fleischer, R. L. and Paretzke, H. G. Method for locating
and characterizing nuclear sources. J. Appl. Phys. 53(6),
4501–4502 (1982).
8. Harvey, J. R. and Weeks, A. R. Recent developments
in a neutron dosimetry system based on CR-39. Radiat.
Prot. Dosim. 20(122), 89–93 (1987).
9. International Atomic Energy Agency. Compendium of
neutron sources and detector responses for radiation
protection purposes. Technical Report Series No. 403
(Vienna: IAEA) (2001).