Optimization of CR-39 for fast neutron dosimetry applications

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 processes. We evaluate the response of the CR-39 to fast neutrons from three sources: ²⁴¹Am---Be, ²⁵²Cf and ²³⁸Pu---Li. Particular attention was paid to background fluctuations that limit the lower detectable dose.     

The effect of etching solution composition on the response of an electrochemically etched CR-39 detector

Etching solutions of different compositions were applied at room temperature (22°C) for electrochemical etching. The background developed during electrochemical etching in a CR-39 track detector was investigated. Detectors irradiated with alphas of 5.49 MeV were measured also. It was found that the PEW solutions (potassiumhydroxid, ethylalcohol, water) showed good sensitivity. One of them (PEW_20/40 was applied for neutrons from a ²⁵²Cf source. The achieved registration sensitivity was about 10⁻⁵ spot/n after 3 hours of etching time.     

Monitoring neutrons from spent reactor fuel by bubble detectors

In order to eliminate the strong temperature-dependence of bubble detectors used for spent fuel assay, a simple way could be to keep them in the water pond but far from fuel assemblies before exposure for about 20 min, until the detectors warm up. Fast neutrons from fuel assemblies in the Paks Nuclear Power Plant, Hungary, were detected by BD-100R type detectors at 28°C (in winter) and at 35°C in summer). Calibration was performed by a standard ²⁵²Cf source in borated water. Burnup monitoring inside fuel assemblies can be provided by smaller diameter detectors prepared from BD-100R type ones.     

Use of CR-39 solid state nuclear track detector in neutron personnel monitoring

Neutron sources like ²⁴¹Am–Be, ²³⁹Pu–Be, ²⁵²Cf and 14.6 MeV neutron generator are being used in oil exploration industries as well as in research institutions. While handling these neutron sources, personnel may be exposed to neutrons. Also personnel working in reactors, accelerators may receive dose from neutrons. These exposed individuals need to be monitored regularly for measurement of neutron doses. The individual neutron doses can be estimated by using Kodak NTA films and CR-39 Solid State Nuclear Track Detector with a polyethylene radiator to increase sensitivity in front in holder. Nearly 1450 personnel are being monitored regularly throughout the country on a quarterly basis. In India, the monitoring system adopted for individual neutron dose estimation having energy from 100 keV and above is described in this paper. Background counts of 0.20 mSv could be measured with CR-39 SSNTD foil system and it has been successfully introduced for Fast Neutron Personnel Monitoring for the country.     

Activation energy of etching for CR-39 as a function of linear energy transfer of the incident particles

In this work, we have studied the effect of the radiation damage caused by the incident particles on the activation energy of etching for CR-39 samples. The damage produced by the incident particle is expressed in terms of the linear energy transfer (LET). CR-39 samples from American Acrylic were irradiated to three different LET particles. These are N (LET₂₀₀ = 20 KeV/μm) as a light particle, Fe (LET₂₀₀ = 110 KeV/μm) as a medium particle and fission fragments (ff) from a ²⁵²Cf source as heavy particles. In general the bulk etch rate was calculated using the weight difference method and the track etch rate was determined using the track geometry at various temperatures (50–90 °C) and concentrations (4–9 N) of the NaOH etchant. The average activation energy F_b related to the bulk etch rate v_b was calculated from ln v_b vs. l/T. The average activation energy E_t related to the track etch rate v_t was estimated from ln v_t vs. l/T. It is shown that activation energy of etching is a constant value for CR-39 detector where E_t was found to be independent on the damage produced by the incident particle.     

Post-irradiation sensitization of CR-39 track detector in carbon dioxide atmosphere

The effect of post-irradiation treatment of CR-39 track detector in carbon dioxide atmosphere on the alpha particle registration sensitivity was investigated. Significant increase in etch rate ratio for 6.1 MeV ²⁵²Cf alpha particle was observed. The sensitization increasedboth as a function of trating time and as a function of carbon dioxide pressure in the treating vessel. Energy dependence of the sensitization was found to be small in the 2–9 MeV alpha particle energy interval. Fading of latent tracks after the sensitization process was slow in a one day period. Pre-irradiation treatment in carbon dioxide showed also some sensitization, though to a lesser extent than post-irradiation treatment. However, exposing CR-39 alpha particles in pure carbon dioxide atmosphere resulted in dramatic decrease in sensitivity. The role of dissolved oxygen and carbon dioxide in the primary latent track formation and in post-irradiation latent track transformation is discussed. Potential influence of the application of sensitization of CR-39 in radon, neutron and cosmic ray charged particle dosimetry is also discussed.     

~(252)Cf自发裂变中子发射率符合测量的回归分析

~(252)Cf同位素源具有标准的自发裂变中子能谱,但由于其半衰期较短,应用中常需要对源强进行标定修正.随着源年龄增加,来自源中~(250)Cf和~(248)Cm自发裂变的影响愈加凸显,不能简单按~(252)Cf的衰变规律计算源中子发射率,而通过锰浴活化的间接测量方法周期较长,且在源强低于10~4 n/s时误差较大.最近,基于中子多重性计数的源强绝对测量算法已得到验证.本文进一步从点模型假设的测量方程出发,在将符合计数率与总中子计数率关联的基础上,分别对符合计数率随源位置、符合门宽的变化关系进行回归分析,提取变化过程的特征系数,建立了两种避规效率变化的~(252)Cf中子发射率测量方法,并基于JCC-51型中子符合测量装置开展实验验证.结果表明:两种回归分析方法的测量值均与标称值的修正结果在2%的偏差范围内一致;反推求得装置中轴线上的探测效率也与基于MCNPX程序的蒙特卡罗模拟计算值相符.研究结果可为活度信息不明的~(252)Cf源强标定及符合测量装置的效率刻度提供便携准确的实验方法.     

A joint UAB-IReS-IPNO neutron comparison exercise with nuclear track detectors

The response of PN3 and CR-39 personal dosemeters with different configurations, developed by the IReS (Strasbourg), the IPNO (Orsay) and the UAB (Barcelona) groups, is investigated in this study. Both dosemeters were mounted on a water-filled phantom and were simultaneously exposed under different incidence angles (0, 30 and 60) to the following: (i) three ISO neutron sources (²⁴¹Am-Be, bare ²⁵²Cf and moderated ²⁵²Cf with Cd shielding), and (ii) two realistic neutron sources (SIGMA and moderated ²⁵²Cf) at the IRSN (Cadarache) facilities. After irradiation, the plastic detectors were etched and evaluated according to local routine procedures and corrections for the effect of source-to-detector distance were taken into account. A comparison of the average background, the minimum detectable dose equivalent and the field calibration factor is performed as well.     

Measurement of nanosize etched pits in SiO2 optical fiber conduit using AFM

Fission fragment tracks from ²⁵²Cf have been observed in SiO₂ optical fiber, using an atomic force microscope (AFM), after a very short chemical etching in hydrofluoric acid solution at normal temperature. The nuclear track starting and evolution process is followed by the AFM direct measurements on the material surface and beyond a fine layer of the surface material. The images of the scanned cones were determined observing the two predominant energies from ²⁵²Cf fission fragments and the development of the tracks in the 150 μm diameter optical fiber conduit.     

System for calibration of track detectors used in gaseous and solid alpha radionuclides monitoring

A laboratory system for the calibration of track detectors and charcoal detectors used in monitoring of radon and its decay products/their aerosols in air, is proposed. The system consists of three main components: (i) the alpha exposure chambers, including alpha monitoring devices and the connection with the ²²⁶Ra radioactive source. The CR-39 track detectors are mounted in the monitoring devices pre-equipped or not with paper filter; (ii) the calibrated  ²²⁶Ra source. Among the three tested sources: ²²²Rn, ²²⁶Ra+²²²Rn and ²²⁶Ra, the ²²⁶Ra source is considered the most appropriate radon source for our calibration system. It is kept into an airtight flat bottom flask, the radionuclide ²²⁶Ra being always in the radioactive equilibrium with their descendants. In the alpha exposure chambers, the source assures the radon at a constant rate; (iii) the ALFAUURASE program for the computation of radioactive accumulation of the alpha ²²⁶Ra descendants. For any initial mass of the parent, the amount and the activity of each alpha decay product and of all the decay products can be calculated by this computation program. Each component of the calibration system is described in the paper. The use of the system for the calibration of CR-39 track detectors in radon measurements is tested.     

Application of CR-39 for alpha-autoradiography and in vivo detection of B accumulations in tumor bearing mice

It is required to achieve an accurate measurement of ¹⁰B distributions and concentrations in the tumor cells for boron neutron capture therapy (BNCT). We employed a technique of neutron capture autoradiography (NCAR) of the whole body samples of tumor bearing mice using CR-39 plastic track detectors to the measurements of ¹⁰B accumulations in mice. In order to confirm the validity of the NCAR measurements, the differential REL spectrum for the neutron-induced particles emitted from the standard filter paper sheets was compared with that for ¹⁰B-compound solution. Differential REL spectrum for protons originated from the biogenically abundant nuclides through ¹⁴N (n, p)¹⁴C and ¹H (n, n′) ¹H reactions was measured in vivo using a small piece of CR-39 inserted into the tumor of mouse.     

Dosimetry of 40 and 70 MeV/n O beams

Using CR-39 plastic track detectors the range values of ¹⁶O ions at two different energies (initially in the beam line, 39.97 MeV/n and 69.98 MeV/n) were measured after escaping the beam pipe and found to be (3050 ± 40) μm and (8210 ± 90) μm, respectively. The longitudinal and projected angular spread of oxygen ions of an initial energy of 69.98 MeV/n in the region of the Bragg peak was derived from the measured geometrical parameters of tracks. Based on a calibration curve (etch rate ratio vs total linear energy transfer in CR-39) and the measured track length distribution at the range end of oxygen ions, the complete depth dose profile of a 67.7 MeV/n ¹⁶O beam in CR-39 (plateau, extended Bragg peak and residual ionization caused by projectile like fragments) was obtained.     

Investigation of nuclear reaction products by atomic force microscopy

The use of Atomic Force Microscope (AFM, from Corporate Head, Santa Clara, California, USA) opened a new way to study latent nuclear tracks. In our experiments we used plastic track detectors of the type CR-39 (Columbia Resin No. 39) Impinging ions with energy above a threshold of 180 keV can alter the molecular structure forming latent tracks. Since nuclear latent tracks have diameters in the range of 10 to 1000 nm, they can be visualized by AFM with a slight chemical etching (6 min in 6 n NaOH solution at 70 °C). These tracks are significant for the energy, momentum and the mass of the incoming particles. In our study, passive CR-39 detectors were irradiated by secondary particles produced bombarding ¹⁰³Rh by ¹⁶O and ¹²C in a wide range of energy (1 MeV/amu to 33 MeV/amu) at the MP Tandem generator of the Laboratorio Nazionale del Sud in Catania, Italy. The experiment was carried out in order to identify the secondary particles and to determine their density and the spatial distribution.     

Performance of CR-39 with addition of DOP (dioctylphthalate) for fast neutron dosimetry

The ENEA fast neutron dosemeter is based on a planar poly allyl diglicol carbonate (PADC) placed in a polyethylene holder. The present paper reports the results of an experimental study of a CR-39^® material with the addition of 0.1% of dioctylphthalate (DOP) produced by the Italian company Intercast Europe S.p.A.

The etching procedure is: pre-etching with 40% KOH water solution 6.25 N and 60% ethyl alcohol at 70°C followed by 12 h of etching in 6.25 N KOH water solution. For the energy dependence of response, dosemeters have been irradiated with neutron sources (²⁴¹Am–Be, ²⁵²Cf, Pu–Li) and 14.9 MeV monoenergetic neutrons. The dosimetric performance of the material for fast neutrons is expressed in terms of sensitivity, background value, lowest detectable dose and energy dependence of response. Moreover, the results of a quality acceptance test of the material, performed on 11 sheets (980×980 mm², 1.4 mm thick) of the same production batch, are given. Therefore, the homogeneity of the neutron sensitivity and of the background signal within a sheet and the whole batch is considered. The results are compared with the acceptance test outcome for a CR39 standard material batch.     

Application of CR-39 detectors for study of corpuscular emission from Prague capillary pinch

The paper describes experimental studies of the corpuscular emission from fast Z-pinch discharges, which were performed within the CAPEX capillary pinch facility in Prague, Czech Republic. Time-integrated measurements were carried out with an ion pinhole camera equipped with CR-39 nuclear track detectors. Irradiated detectors were etched at the standard conditions, and developed tracks were analysed with an optical microscope coupled with a CCD camera. It was found that the fast capillary discharges emit strong corpuscular streams. On the basis of the optical analysis of the etched detectors it was estimated that the time-integrated particle flux, at the distance of 20 cm from the collimator outlet, was about 3.5×10⁷ particles/cm²/pulse. Particular attention was paid to analysis of ion-track photos, which were obtained by means of an electron microscope. Details of the ion micro-craters have been observed in the photos of fractures of the CR-39 detectors after their 7 h etching.     

Calibration study on the triton response of CR-39 track detector

Triton response of the CR-39 track detector has been studied at energy ranges below 2.7 MeV. Triton irradiation was made both on the top and the well polished side surface of the CR-39 sample sheets, using ⁶Li(n,t)⁴He reaction in a thermal neutron field. At large residual ranges more than 10 μm, fine results of etch rate ratio were obtained by analysing the growth curves of etch-pit radius on the top surface. But the response at near the track end-point could not be obtained well in this method, as a result of the missing track effect. Clearly resolved response at short residual ranges was attained by means of the shape analysis of the etch-pit profile observed on the side surface.     

Modifications in track registration response of PADC detector by energetic protons

It has been well established that different ionising radiations modify the track registration properties of dielectric solids. In an effort to study the response of Polyallyl diglycol carbonate (PADC Homalite) detector towards fission fragment, PADC detectors were exposed to 10⁴ Gy dose of 62 MeV protons and then one set of samples were exposed to fission fragments from a ²⁵²Cf source. Two of these detectors were containing a thin layer of Buckminsterfullerene (C₆₀). The study of the etched tracks by Leitz Optical Microscope reveals that the track diameters are enhanced by more than 70% in the proton irradiated zone as compared to that in the unirradiated zone. Scanning Electron Microscopy was performed after etching the sample in 6 N NaOH at 55°C for different etching times, to study the details of the surface modifications due to proton irradiation of PADC detectors with and without C₆₀ layer. Our observations revealed that the diameters and density of proton tracks have increased with etching time on the surface facing the fullerene layer as well as the other surface. However, a relatively more open structure of the etched surface containing C₆₀ as compared to the bare one may be an indication of the extra damage caused by the energy released upon the destruction of C₆₀ molecules by energetic protons.     

Registration temperature effect on sensitivity of CR-39(DOP) and SR-90 polymer track detectors

The samples of CR-39(DOP) and SR-90 polymer track detectors have been exposed to -particles from ²⁴¹Am source in an exposure unit. The temperature of the detectors during irradiation has been varied from −30°C to 70°C. These exposed samples have been etched in 6.25 N NaOH solution at 60°C for various etching times. The variation of sensitivity of these detectors as a function of registration temperature has been studied. It has been observed that at the fixed registration temperature, the sensitivity of SR-90 is more than CR-39(DOP) polymer track detector. However, the enhancement in sensitivity with the decrease in registration temperature is more pronounced in case of CR-39(DOP) than SR-90.     

Track etch rates along the trajectories of nitrogen and oxygen ions in CR-39

Experimental studies on track etch rates in CR-39 performed with protons, deuterons and alpha particles as well as ⁷Li, ¹¹B and ¹²C ions were extended to ¹⁴N and ¹⁶O ions. The results are compatible with the general systematics found for the dependence on the kind of ion and its initial energy. Analysing the etch rate ratios as function of the restricted energy loss (REL), the non-existence of a unique relationship has been confirmed. However, assuming a dependence of the etch rate ratio not only on REL, but also on the depth within the detector where a given REL value occurs, all experimental data could be adjusted. The experiments with ¹⁴N and ¹⁶O ions allow extension of the REL range studied up to about 14 000 MeV/cm. The whole area relevant to neutron-induced charged particles generated within the CR-39 detectors is covered thereby. Having added the data for ¹⁴N and ¹⁶O ions, the array of curves for the etch rate ratio could be expanded up to 14 000 MeV/cm without inconsistencies, demonstrating the compatibility of the new data set also quantitatively.     

Observation of the reaction products formed in the interaction of 3.65 A GeV O ions with thick copper target at wide angles

Experiments have been carried out to study the ‘heavy fragments’ emitted at wide angles in the interaction of 3.65 A GeV ¹⁶O ions with a thick Cu target, using a stack of CR-39 track detectors. Diametric distribution in a stack registering ¹⁶O-beam halo are compared with diameters observed in a stack placed downstream at an angle of 25°. There is a strong indication that the heavy fragments are scattered at large angles.