Nuclear track radiography of “Hot” aerosol particles

Nuclear track radiography was applied to identify aerosol “hot” particles which contain elements of nuclear fuel and fallout after Chernobyl NPP accident. For the determination of the content of transuranium elements in radioactive aerosols the measurement of the -activity of “hot” particles by SSNTD was used in this work, as well as radiography of fission fragments formed as a result of the reactions (n,f) and (γ,f) in the irradiation of aerosol filters by thermal neutrons and high energy gamma quanta. The technique allowed the sizes and alpha-activity of “hot” particles to be determined without extracting them from the filter, as well as the determination of the uranium content and its enrichment by ²³⁵U, ²³⁹Pu and ²⁴¹Pu isotopes. Sensitivity of determination of alpha activity by fission method is 5×10⁻⁶ Bq per particle. The software for the system of image analysis was created. It ensured the identification of track clusters on an optical image of the SSNTD surface obtained through a video camera and the determination of size and activity of “hot” particles.     

The measurement of the fragment emission angles in the reactions of <135 MeV/u C and O in tissue equivalent targets

Different stacks of tissue equivalent targets interleaved with CR-39 nuclear track detectors were irradiated with 135 MeV/u ¹²C and ¹⁶O ions. After track etching and measurement by an automatic image analysis system, a method of trajectory tracing was applied. The trajectories of particles were reconstructed using a pattern-matching method based on a comparison of relative track coordinates.

Fragmentation products have a lower charge and can be clearly distinguished by their smaller track sizes. The track positions within the individual trajectory are additionally fitted to a straight line, from which we can determine the direction of the traversing ion within a path of a few mm. We performed an angular distribution study of the fragments, which we compared to simulation results obtained by a simple particle emission model. For the fitted parameters the model showed agreement within the margins of error but failed to describe the energy dependence and thus should be further improved and upgraded.     

Verification of radioactive equilibrium to discriminate radon and progeny with LR 115 under a thin film geometry

A system of image analysis is applied to the track analysis of a plastic detector (LR 115). Based on track characteristics the system permits the separation of tracks produced by ²²²Rn and ²¹⁸Po from those produced by ²¹⁴Po. LR 115 was used inside a thin film geometry monitor and irradiated under very low ventilation conditions, where secular radioactive equilibrium between radon and progeny is expected. The monitor is used intending to exclude the entrance of external radon progeny in the sensitive volume of the plastic detector. The radioactive (secular) equilibrium is rapidly attained inside the monitor and equal numbers of particles from ²¹⁸Po, ²¹⁴Po and ²²²Rn are expected to reach the plastic. In order to guarantee good detection efficiency in the restricted volume, and to discriminate alpha energies, the LR 115 piece inside the monitor is covered with an aluminum foil of suitable thickness. The separation of tracks produced by alpha particles of different energies is made through the use of two track parameters related to area and opacity of the tracks. The ratio of tracks produced by (²¹⁸Po and ²²²Rn) and ²¹⁴Po—expected as two—is used to test the separation method in a series of controlled irradiations. Results point to the experimental attainment of radioactive equilibrium inside the monitor supporting the determination of ²¹⁴Po concentration alone, and points to an exclusive entrance of ²²²Rn inside the monitor, at low ventilation rates. This way, in situations where radioactive equilibrium inside the monitor may be considered, the exclusive measurement of radon concentration in the environment is possible.     

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.     

Determination of isotopic composition of plutonium in hot particles of the Chernobyl area

The knowledge of the isotopic composition of man-made transuranium elements (TUE) in the environmental samples is of great interest because, on the basis of these data, statements about the origin of the TUE can be made. One of the most radiotoxic elements released during reactor accidents and nuclear weapons tests was plutonium with the alpha emitters ²³⁸Pu, ²³⁹Pu, ²⁴⁰Pu, ²⁴²Pu and the beta-emitter ²⁴¹Pu which decays into ²⁴¹Am. The determination of plutonium in “hot” particles from the Chernobyl reactor was accomplished by means of solid state nuclear track detectors registering the alpha particles and by alpha spectroscopy after chemical treatment. Furthermore, in order to perform a complete analysis of the isotopic composition one of the “hot” particles has been investigated by resonance ionization mass spectrometry which possesses an excellent sensitivity and a good isotopic resolution.     

Computation of etched track profiles in CR-39 and comparison with experimental results for light ions of different kinds and energies

Computation of etched track profiles needs the knowledge of the variable track etch rates along the ion trajectories. Using the depth-dependent track etch rates experimentally determined for perpendicularly incident protons, deuterons and alpha particles as well as ⁷Li, ¹¹B, ¹²C, ¹⁴N and ¹⁶O ions of different energies simulations of the track development were performed. Two models of track etching were applied for that purpose recently published in literature. Although the models are based on the same physical fundamentals the results are slightly different. The reasons of the discrepancies were found by analysing the algorithms in detail. Comparison of the calculated track profiles with those determined experimentally from longitudinal sections of the etch pits showed good agreement for non-overetched as well as overetched tracks. The consistency of the whole experimental data set was checked by analysing the correlation of the track etch rates with geometric track parameters for all kinds of ions and etching times covered by the experiments.     

Angular and dose dependence of CR-39 neutron response for shape-selected tracks

A shape selection method corresponding to an energy discrimination was used to eliminate unwanted events disturbing evaluation of CR-39 detectors in detecting tracks induced by particles both of perpendicular and oblique incidence. The angular dependence of the response was examined, detecting fast neutrons from ²⁵²Cf with shape selection technique at various angles and distances. Also, the CR-39 track detectors with the ²⁵²Cf source were exposed to high γ-intensity of a ⁶⁰Co irradiation facility in the range 0.1 to 4.5 kGy, similar to the exposures inside spent fuel assemblies. Using the two functions the lower limit of burnup could be determined by the method.     

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.     

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.     

Neutron production in extended Cu-target irradiated with relativistic C-ions at Dubna, as studied with SSNTD and nuclear chemistry

An extended Cu-target was irradiated with 22 and 44 GeV carbon ions. The target was in contact with a (CH₂)_n-block for the moderation of secondary neutrons. Small holes in the moderator were filled with either lanthanium salts or uranium oxide. The reaction ¹³⁹La (n,γ) ¹⁴⁰La was studied via the decay of ¹⁴⁰La (40 h), and the reaction ²³⁸U (n, γ) ²³⁹U ²³⁹Np was studied via the decay of ²³⁹Np (2.3 d). In addition, a variety of solid state nuclear track detectors (SSNTD) were used. Results will be presented. The yields for the formation of (n, γ) products agree essentially with other experiments on extended targets carried out at the Synchrophasotron LHE, JINR (Dubna). To a first approximation, the breeding rate of (n, γ) products, as well as the specific track density, seen with several SSNTDs, doubles when the carbon energy is increased from 22 to 44 GeV. If, however, results at 44 GeV are compared in detail to those at 22 GeV, we observe an excess of (37 ± 9) % in the experimentally observed ²³⁹Np-breeding rate over theoretical estimations. Experiments using solid state nuclear track detectors are giving similar results. We also observed in the past such excess in the yield of other secondary particles in relativistic heavy ion interactions above a total energy of approximately 35–40 GeV.     

SSNTD and radiochemical studies on the transmutation of nuclei using relativistic ions

Extended targets were irradiated for transmutation studies with relativistic heavy ions. For this, a metal core was surrounded by a paraffin moderator. The metal is either copper or lead and it was irradiated with deuterium, alpha, or carbon beams of 1.5 or 3.7 GeV/u at the SYNCHROPHASOTRON, LHE, JINR, Dubna, Russia. During this irradiation copious amounts of secondary neutrons are produced and studied with SSNTD detectors and radiochemical sensors, for example ¹³⁹La (n, γ) ¹⁴⁰La→β⁻. The yield of reaction products allows an estimation of secondary neutron fluxes. The yields of all kinds of reactions produced with deuterium and alpha beams obey to some extent the law of “limiting fragmentation”, i.e. they show little influence on the energy and the kind of incoming particles. However, one observes with 44 GeV ¹²C ions always enhanced nuclear cross-sections induced by secondary particles. This behavior could not be confirmed with theoretical estimations based on the Dubna Cascade Model in its Cascade Evaporation Model version (DCM-CEM). Finally, some results for transmutation studies on ¹²⁷I and Cu will be presented.     

Track structure in dielectric and semiconductor single crystals irradiated by heavy ions with high level of inelastic energy losses

The phenomenological model of the track formation processes during a heavy ion passing through materials is discussed. This model is based on the scanning tunneling and electronic microscopy investigations of diamond single crystals and stainless steel subjected to ⁴⁰Ar, ⁸⁴Kr and ¹²⁹Xe ion irradiation with energies in the MeV region. The energy and temperature criteria when crater formation on the surface during the heavy ion irradiation takes place are introduced.     

Boron determination in tourmaline by neutron induced radiography

The technique of neutron induced radiography has been applied to determine the boron concentration and its spatial distribution in mineral tourmaline collected from Swat Tourmaline Granite, Northern Pakistan. The technique involves the simultaneous irradiation of sample and a standard fixed on a track detector with thermal neutrons and the counting of alpha and ⁷Li tracks produced in the detector from the nuclear reaction ¹⁰B(n,)⁷Li. Boron concentration is determined by comparing the ⁷Li and alpha particle tracks density with that of a standard of known boron concentration. Boron concentration in tourmaline has been found to be (3.40±0.01)% in this study which is on the upper side within the normal range (2.5–3.8)% reported in the world. The presence of somewhat higher concentration of boron in tourmaline indicates that the Swat Tourmaline Granite was generated as a late stage hydrothermal activity during the Himalayan Orogeny.     

400 AMeV 12C诱发乳胶核反应重电离粒子前后关联研究

对400 AMeV 12C诱发乳胶核反应重电离粒子的前后关联进行了研究。重电离粒子来源于靶核碎片,分为灰径迹粒子和黑径迹粒子两种。实验结果很好地验证了核-核碰撞几何模型。灰径迹粒子的发射在前、后半球是各向异性的,而黑径迹粒子的发射基本是一致的。向前、向后发射的灰径迹粒子、黑径迹粒子平均多重数对重电离粒子数n_h呈线性依赖,黑径迹粒子、灰径迹粒子的向前发射随n_h的增加而增加的幅度分别大于其向后发射随n_h的增加而增加的幅度,但核内级联效应受靶核大小的影响,向后半球内发射的灰径迹粒子平均多重数随n_h的增加有饱和现象,这些多重数关联特性基本上可以利用基于碰撞几何的旁观体-反应体模型及级联蒸发模型来解释。The forward-backward multiplicity correlation of heavily ionized particles produced in 12C-emulsion interactions at 400 AMeV is investigated. The heavy ionized particles, come from the target fragments, are divided into grey track particle and black track particle. The experimental results can be well explained by the geometry model of the nucleus-nucleus collisions. The emission of grey track particles in forward and backward hemisphere is not isotropic, but the emission of black track particle is almost isotropic. The averaged multiplicity of grey track particles and black track particles in forward and backward hemisphere linearly depend on the number of heavily ionized particle n_h, the correlation strength in forward hemisphere is greater than that in backward hemisphere, but the dependence of grey track particle in backward hemisphere on the number of heavily ionized particle n_h shows the saturation because of the intranuclar cascade effect is influenced by target size. The characteristics of multiplicity correlations can be well explained by the participant-spectator model based on the colliding geometrical picture and the cascade evaporation model of high energy nucleus-nucleus collisions.     

Decay Analysis of Ge Isotopes Formed in Reactions Induced by Tightly and Loosely Bound Projectiles

The dynamical cluster-decay model (DCM) is employed to investigate the decay of ^68,70Ge^* compound nuclei formed respectively via tightly (⁴He) and loosely (⁶He) bound projectiles, using ⁶⁴Zn target. The study is carried out over a wide energy range (E_c.m.~5 MeV to 16 MeV) by including the quadrupole deformations (β2i) and optimum orientations (θ_i^opt) of the decaying fragments. The fusion cross-sections, obtained by adding various evaporation channels show nice agreement with the experimental data for ⁴He+⁶⁴Zn reaction. The contribution from competing compound inelastic scattering channel is also analyzed particularly for ⁶⁸Ge^* nucleus at above barrier energies. On the other hand, the decrement in the fusion cross-sections of ⁷⁰Ge^* nuclear system is addressed by presuming that ⁶⁵Zn ER is formed via two different modes:(i) the αn evaporation of ⁷⁰Ge^* nucleus, and (ii) 1n-evaporation of ⁶⁶Zn^* nuclear system, formed via breakup and 2n-transfer channels due to halo structure of the ⁶He projectile. Besides this, the suppression in 2np evaporation cross-sections suggests the contribution of another breakup and transfer process of ⁶He i.e. ⁴He+⁶⁴Zn. The contribution of breakup+transfer channels for ⁶He+⁶⁴Zn reaction is duly addressed by applying relevant energy corrections due to the breakup of " ⁶He" projectile into 2n and ⁴He. In addition to this, the barrier lowering, angular momentum and energy dependence effects are also explored in view of the dynamics of chosen reactions.     

Determination of the range of alpha particles in SSNTD by optical density method

A technique based on the optical density (D) measurement of the etched track is useful for charged particles spectroscopy using SSNTD. It was shown that the stopping power of alpha particles in CR-39 is proportional to D. We measured the optical density and derived an expression to estimate the range of alpha particles in CR-39 detector as a function of the bulk etching rate and etching time. The relation between the etching time, track parameters (depth, radius) and D for different alpha particles energy and etching conditions were studied. A relation describing D as a function of track size is proposed.     

Heavy-ion particle spectrometry by track pattern in muscovite detectors

Muscovite mica detectors were irradiated with the ions: ¹⁹F of 47.5 MeV, ²⁴Mg of 57 MeV, ²⁸Si of 28 and 74 MeV, ³²S of 32 and 74 MeV, ⁶³Cu of 78.75 MeV and with neutron induced uranium fission fragments. Using optical microscopy, after an appropriate chemical etching, two characteristic etched track structure patterns were observed: a rhombic pyramid terrace structure for the Mg, Si and S ions, and a rhombic prism structure for the Cu ions and fission fragments. The use of these etched track patterns to discriminate two groups of ions between them, for the energy range covered in this work, is proposed.     

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.     

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.     

Nucleon-nucleon final-state interactions in the reactions He(p, d)2p, He(p, t)2p and He(p, He)pn

The energy spectra of deuterons, tritons and ³He particles from the reactions ³He(p, d)2p, ⁴He(p, t)2p and ⁴He(p, ³He)pn have been measured at angles between 6° and 60° lab. The ³He(p, d)2p reaction was studied at both 30.5 and 49.5 MeV incident proton energies, while the other two reactions were studied at 49.5 MeV only. The energy spectra are compared with calculations based on the Watson-Migdal model of final-state interactions.