NW/. Tracks Radial. Meas., Vol. 14, No. 3, pp. 373-378, 1988 0191-278X/88 $3.00 +O.

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Int. .I. Radial. Appl. Instrum., Part D Pergamon Press plc
Printed in Great Britain

THE CRITICAL ANGLE DEPENDENCE OF CR-39
NUCLEAR TRACK DETECTORS FOR 3-10 MeV PROTONS
AND 7-15 MeV ALPHA PART!CLES

P. M. STAFFORD,J. L. HORTONand K. R. HOGSTROM
Department of Radiation Physics, The University of Texas M. D. Anderson Hospital and Tumor
Institute at Houston, Texas, U.S.A.
and
P. M. DELUCA, Jr* and D. HOL~LIN~
*Department of Medical Physics and TDepartment of Physics, The University of Wisconsin,
Madison. U.S.A.

(Received 5 October 1987; in revisedform 3 March 1987)

Abstract-With the advent of routine clinical usage of fast neutrons as a radiation therapy modality,
interest in the solid state nuclear track detector CR-39 as a possible in vivo neutron dosimeter has
increased. One facet of the problems associated with this application is the calibration relationship of the
linear energy transfer (LET) of a charged particle and the normal incidence diameter of the etch pits found
in CR-39 after exposure and subsequent etching. This study, performed on a tandem electrostatic
accelerator at the University of Wisconsin, Madison, provides such a calibration for both critical angle
and normal incidence diameter versus linear energy transfer for several incident energies of proton and
alpha particles. Plots of detection efficiency versus angle of incidence for 3, 6, and 10 MeV protons, and
7, 10, and I5 MeV alpha particles are used to determine the critical angle of each particle and energy.
The bulk etch and track etch rates were determined by a &i-squared minimization calculation based upon
published relationships and the measured major and minor axis dimensions obtained at each angle of
incidence, particle and energy. Results of normal incidence diameter versus LET measurements show a
smooth monotonically increasing curve with LET. A bulk etch rate of 1.32 pm/h for a 16 h etch in 6.25 N
NaOH was measured.

1. INTRODUCTION 2. METHODS AND MATERIALS
OF THE charged particles created by fast neutrons The CR-39 used to perform these measurements
interacting with tissue, protons and alpha particles was specially formulated by American Acrylics
provide greater than 90% of the dose (Wells, 1978). and Plastics (Stratford, Connecticut, U.S.A.) for
The solid state nuclear track detector (SSNTD) CR- use as a nuclear track detector material, and was
39 can be used to detect these particles, subject to the supplied in sheets 0.635 mm thick. The material was
restrictions of critical angle and linear energy transfer cut to 2.5 x 7.6 cm for ease of handling in the image
(LET). The critical angle is defined as the angle of analysis system.
incidence of a particle at which the surface normal The exposures were performed at the University of
component of the track etch rate equals the rate of Wisconsin tandem electrostatic accelerator which is
removal of the detector surface, or the bulk etch rate. capable of accelerating protons to an energy of
At this angle, no visible track is obtained by the 10 MeV and alpha particles to an energy of 15 MeV.
etching process. Tracks are created in CR-39 by The beam passed through a 90” bending and ana-
damage to the polymer by incident charged particles. lyzing magnet (Fig. 1) and thence to a 1 m dia.
This damage can be visualized by chemical etching to scattering chamber. At the scattering chamber, the
forms pits, measurable by an optical image analysis beam was collimated to a 1 x 2 mm spot which then
system. The size of the pit major and minor axes are impinged upon a 1058 pg/cm’ Ta target positioned
determined by the LET and angle of incidence to the normal to the incident beam. Two identical col-
detector surface of the impinging particle. The cali- limation systems were placed symmetrically about the
bration of CR-39 as a function of varying LET and particle beam direction. Each system consisted
angle of incidence for protons and alpha particles is of three double collimators with 1 x 10 mm front
the subject of the research described below. and 3 x 30 mm rear slits. The front slit was

Requests for reprints should be addressed to: Patrick M. Stafford, Ph.D., Department of Radiation Therapy, Fox Chase
Cancer Center, Central & Shelmire Avenues, Philadelphia, PA 19111, U.S.A.

373

4 cm apart. detector surface. 0” being each scattering direction at the location of the CR-39. L2 _ Electrostatic lenses L4 Pl. + 50”. with three irradiations required at By measuring the response of this detector relative to each energy for each particle to span the range of those located at the position where the CR-39 was incident angles from O-85”. and the slits were particles of 7.6. 4. and 10 MeV. as shown in Fig. 1. The irradiations provided positioned. Schematic diagram of the University of Wisconsin. Figs 2 and 3. fabricated to fit onto the baseplate of the three-slit The scattered fluence was measured with 1500 pm collimator assembly as shown in Fig. Madison tandem electrostatic accelerator facility. Six detectors were irradiated at one time the plane containing the beam and other detectors. Beam monitor detector POLARIMETER FIG. . mean angles of & 40”. used for these measurements. This number was chosen to yield The geometry of this calibration is illustrated in adequate statistics while minimizing track overlap. 2). M2_ 90” Electrostatic mirrors Dl-D6 _ Magnetic beam steerers Ll.2cm from the target spot. SM Beam switching magnet Sl-s4 1 Metered beam centering and defining slits T _ Target D __ Three detector collimator M . normal incidence to the collimated Coulomb scat- Another surface barrier detector was fixed 15” below tered beam. 10. while the surface barrier monitor chamber was fixed 15” below the plane of the beam and the other detectors. Schematic diagram of the one meter diameter scattering chamber. M. Protons of 3. STAFFORD et al Sl I I 90” MAGNET TANDEM ACCELERATOR ____-___-’ ION SOURCE \ 1’ \ Ml.314 P. P2 _ Precession solenoids C Terminal carbon-foil stripper CZl D6 L3. L4 II Magnetic quadrupole lenses s3 -. 2. and + 60” with respect Custom holders for the CR-39 detectors were to the bombarding particles (Fig. 5. The CR-39 thick silicon surface barrier detectors positioned at detectors were irradiated at 5” increments. Scattered particles were detected at were used for this experiment. and alpha The exposed track detectors were etched for 16 h in FIG. and 15 MeV incident on the target 15. it was possible to infer the scattered 2 x 103-3 x lo3 tracks per square centimeter on the fluence when the CR-39 was in place. 25. The Ta target was suspended from the lid of the chamber.

12 cm’ for major and minor axis deter- . The detectors were scanned by a Joyce-Lobe1 using volumetric flasks and a precision balance for Nikon Magiscan 2A image analysis system over an control of the etchant preparation. a filtered.25 N NaOH. FIG. Each batch detectors. Each position allowed indexing of the detector in 5” increments. main. while the monitor chamber can be seen at the far right. 3. 4. CR-39 detectors in custom holders. Approximately area of 0.OYC. 21 pm of surface thickness were removed from the tained at a temperature of 70” + O. Calibration of the collimation system with surface barrier detectors (square blocks behind the collimators). CRITICAL ANGLE DEPENDENCE OF CR-39 DETECTORS FIG. The metered beam defining slit assembly is at the left of the chamber. circulating bath of 6. of detectors was etched in freshly prepared NaOH.

6.09 The critical angle determination and efficiency measurements were performed by measuring the Alpha/ 15 52.38 & 1.29 * 0.35 Alpha/l0 75. the observed efficiency of appropriate monitor-to-detector ratio as mentioned detection for this study was not 100 percent. Proton/6 8. Because of the small (3 pm) size of normal incidence diameter. Normal incidence diameter versus LET. . STAFFORD et al FIG.80 3.23 number of tracks over 0.2. -0 20 40 60 60 100 LET (k&J/pm) 3.86 7.1. The monitor chamber and exit port for the Faraday cup may be clearly seen on the right.74 scattered particles. CR-39 detectors in place for irradiation. M.04 F 1.1. although in the calibration procedure above.and diameter versus LET using equation (2) to transform VT to IO-MeV protons.70 24. We have reproduction of position. The 5” intervals did not permit grid slide was also used in this study to permit a precise determination of critical angle.. To ensure accurate reproduction of the Table 1. and the measured normal incidence diameter.10. The numbered it was still very high. The plot of normal incidence diameter versus LET is shown in Fig. 5. Measured parameters for the normal incidence positioning of each successive detector.21 22. The dotted line is a transform of V.55 pm.93 17. a numbered diameter determination grid slide was used to check that the stage had been Normal incidence returned to the correct starting point. Proton and alpha particle critical angle versus energy FIG. mination. 6. the basic building block of CR-39 (Cassou and Benton. half the bulk etch layer thickness. RESULTS 3.38 k 1.13 Proton/3 16. The measured fluence was corrected for detector position by applying the the IO-MeV proton tracks. Normal incidence diameter versus LET The LET or restricted stopping power for CH.7 1 creased over the previous measurements to improve the counting statistics. P. versus LET to normal incidence Figure 7 shows the response of CR-39 to 3-.90 + 1. 3. The detectors Particle/energy LET diameter were scanned only in the area around the central axis (MeV) (keV/p m) Olm) of the collimation system to minimize effects of Proton/l0 5.06 11. 1978). Table 1 uses LET values calculated at a depth of 10. 6.18 cm2. This area was in- Alpha/7 100. was calculated based upon stopping powers from Benton and Henke (1969).

10 and 7 MeV incident on target. 7. The average bulk etch rate from where V = VT/V. t is these calculations was determined to be 1. These extrapolated values may be found in Table 2.1 J major axis profile.4 Alpha/ 15 54.6 Proton/3 16. given by dividing the bulk etch depth by the cosine of the calculated critical angle for that particle.93 1. Figure 8 shows the critical angle response of CR-39 _.2 6 and 3 MeV incident on target. The fact that these efficiency curves do not sharply 0 fall off can be attributed to multiple Coulomb scatter.6 Proton/3 16.88 8. particles near the critical angle were not used due to The following relations for V. a is the major axis dimension. 1980): cos $.06 1.9 Alpha/l0 75.32 pm/h.5 Alpha/7 162. . 10 and 15 MeV. ticles at 15. 1980): mization to obtain an average bulk etch rate..2 44. The LET values shown in Table 2 were calcu- lated for the energy of the particle at the depth in CH.9 Proton/6 8.86 1.) t. Track etch rate versus LET 2 0.2 Proton/l0 5. 9.395 18. 3.342 9.00 13.0 61.4 Alpha/ I 5 52.0 18.336 55.532 30. and FIG. 2 0.8 30.9 Proton/6 9. Registration efficiency versus angle for alpha par- the extrapolated values are listed in Table 2.t $ is the angle J Vcos$ of incidence + 1 of the particle (2) After determination of the track and bulk etch rates.0 55. To optimize this calculation.0 This calculated critical angle may also be found in Table 2.4 critical angle (MeV) (keV/p m) 01$h) (degrees) 5 0.2 estimated the critical angle from the 50% efficiency point of the curves. As can be seen in Figs 7 and 8. Alpha/7 100. The calculated track etch rate values are a function the etch time in hours and: of LET as shown in Table 3 and Fig. CRITICAL ANGLE DEPENDENCE OF CR-39 DETECTORS 371 Table 2.1 where b =2V. From equation (1) and the measured parameters a. and this data one can determine bulk (Vo) and track (V. Calculation of track etch parameters (normal incidence II/ = 0’).9 Alpha/l0 86.6 h Calculated 2 Particle/energy LET Y s 0. = VG/VT (3) 1._ for alpha particles of 7. VG for each particle and energy using equation (2). Measured parameters for the critical angle study Particle/energy LET Extrapolated critical Calculated critical (MeV) (keV/p m) angle (degrees) angle (degrees) Proton/l0 5.54 56.3.80 1. v cos lj . can be determined from the relationship (Somogyi. A computer program was Another method for determining critical angle is to written which calculated V for a given VG using utilize major and minor axis data versus angle. A plot of b versus and for the minor axis dimension (b) of the track II/ was then fit by performing a chi-squared mini- were used for these calculations (Somogyi.866 44. the estimation g Table 3.0 9. b.54 23.70 2.02 49.740 61. the critical angle II/. Registration efficiency versus angle for protons at 10.6 _m ing.2 1 2.71 38. some data for alpha etch rates and the critical angle. The same 0 20 40 60 60 angle to normal (degrees) procedure was used to estimate the critical angle.5 FIG. The J-[&J]i+4[&]?]lii (1) minor axis dimension was chosen for the fit because it could be more accurately measured at higher angles _ r b 1’ of incidence due to elongation and shallowness of the ‘-12v. 8. the etch rate ratio inaccuracies in the major axis data.

Hirh Phys. of 0. This angular response Proton-recoil neutron dosimeter for personnel moni- toring. 9. LA-7288-T. Rome. Oswald R. Schumacher U. c 0 MIllI 5 10 50 100 LET (k&'//m) FIG. has been studied by several investigators for lower Cassou R. The shape of the efficiency versus angle curves is Track Detection 2. (1981) registration does not occur. For any charged particle there is a maximum Instrum. 6) that the normal incidence detectors. since the normal 50% efficiency point to the s-axis will result in a incidence diameter at that energy is near 3 pm. neutron radiotherapy. Nucl. Los Alamos sponding to that of 10 MeV protons. Meth.378 P. 2142. To effectively obtain a higher order fit for normal incidence diameter versus LET. (1978) Properties and applications energies (Benton et al. 10 shows that the critical angle Muhling E. Ph.991. using equation (2) to obtain the dotted line of Fig. M. (1984) Ther- variation changes exponentially with LET. scattering. critical angle to the normal beyond which track Benton E.991). and Wheeler R.. 801-809. The dotted line FIG.8 keV/pm. system. typical of these other investigations. 67.. The straight line Department of Energy Grant DE-FG02-86ER60417. rithm (LET) may be seen in Fig. (1969) Heavy particle range relations for dielectric nuclear track detector. The consistent underestimation of the calculated critical background caused by the etching process makes angle. Frank A. 13th Int. D. 9 (1. = 0. . 1984). An Track Detect&s. Tracks 9. From the practical standpoint of measuring the Wells A. with r =0. Solid Slate Nucl. The dotted is a quadratic fit to the data with a correlation coefficient line is on exponential fit to the data. or 5.. (1980) Development of etched nuclear tracks. 10. and Mrs D. Scientific Laboratory. examination of Fig. 6. is a fit of an exponential function to the data with a correlation coefficient of 0. comitant reduction of the LET of the particle.S.D Dissertation.. 113-I 1I. diameter of the track varies predictably with LET. Instrum. electrochemically etched CR-39 to protons of 10 keV to 3 MeV. (1978)Calculation of dosimetry parameters for fast tracks themselves. transform of this fit of VT versus LET was performed Knutson for use of their laboratory. 1981. 173.993.) versus LET. versus LET data was first performed as the University of Wisconsin accelerator facility is gratefully shown by the dotted line of Fig. monuclear fusion product diagnostic by nuclear track We also conclude (Fig. Track etch rate (I’. This research was supported in part by National Cancer Institute Contract NOl-CM-27531. Nucl. In Proc. REFERENCES 4. A acknowledged. It is hypothesized that this broadening near the tracks smaller than this diameter increasingly difficult point of zero efficiency is due to multiple Coulomb to discern. it would seem that the LET corre. Somogyi G. CONCLUSIONS Benton E. and Benton E. and Paretzke H.. STAFFORD er a! - :. of CR-39 polymeric nuclear track detector. is the limit of detection for CR-39 scanned with of critical angle by dropping a perpendicular from the optical image analysis systems..Calculated critical angle versus log LET. Merh.993. and Ing H. and U. Muhling et al. 173-179. a quadratic Ackrlo~leclgements-The help and expertise of the staff at fit of the V. Casavant for the loan of the assistance with the collimation A plot of the calculated critical angle versus loga. (1985) The response of decreases with the increase in energy and the con. Italy. Arneja A. Nucl.. The critical angle Cross W. 87-92. Thanks also to Professors Paul Quin and L. and Henke R. Nucl. 40. 10. Conf.