A search for superheavy nuclei tracks in extraterrestrial olivine crystals

A study is made for the search of superheavy nuclei in Marjalahti, Eagle Station and in other pallasite olivines. The olivine crystals are calibrated for heavy ion track lengths by using heavy ion beams from cyclotrons. The calibration for ultra heavy ions which are presently not available with sufficient energy to produce volume tracks in olivine crystals, is based on Katz and Kobetich model of track formation. The length spectrum of volume tracks, revealed by puncturing them with focussed Nd-glass laser beam, is measured and the abundances of different nuclei groups are calculated. Partial annealing has been used at 430°C for 32 hr which eliminates the interfering tracks due to nuclei of atomic numberS ≤ 50. During the scanning 4 cm³ olivine crystals, about 360 long tracks of uranium group as well as two very long tracks have been found. If these tracks belong to superheavy nuclei, the relative abundance of super heavies is found to be 6 × 10⁻¹¹ in galactic cosmic rays.     

On search and identification of tracks due to short-lived SHE nuclei in extraterrestrial crystals

The unique approach for search and unambiguous identification of short-lived (T_1/2=10³–10⁷ years) superheavy nuclei in cosmic-ray products of the recent nucleosynthesis in our Galaxy are discussed.It is based on: (a) the ability of non-conducting crystals to register and to store for many million years the tracks due to fast nuclei with atomic number Z20 (“fossil” tracks);(b) calibrations of the said crystals with accelerated heavy ions (20Z92) and on revealing the volume etchable track length (VETL) of the fast nuclei coming to rest inside crystals—both of fossil and “fresh” tracks—to determine the charge distribution of cosmic-ray nuclei tracks and(c) the so-called “four-zone” model of tracks in crystals (and also glasses) which provides not only the VETL track length dependence for 20Z92 nuclei but also demonstrates the regular annealing behavior of VETL of 20Z92 nuclei in a broad temperature interval.This approach was first applied in the early 1980s to investigate the “fossil” tracks due to 22Z92 cosmic-ray nuclei in olivine crystals from meteorites-pallasite Marjalahti and Eagle Station.The discovery of Th–U cosmic-ray nuclei tracks in 1980 was unambiguously confirmed by calibrations of the same crystals with ²³⁸U, ¹⁹⁷Au and ²⁰⁸Pb accelerated ions in the late 1980s. More than 1600 tracks due to cosmic-ray actinide nuclei were measured during the last two decades of the 20th century.Also, 11 anomalously long tracks (track length exceeds by a factor (1.6±0.1) the track length due to Th–U nuclei were measured. The detailed analysis shows that at least 5 of these tracks could not be attributed to the Th–U nuclei. It means that now we have a preliminary proof on the existence Z110 nuclei in cosmic-rays. The abundance is Z110/Th–U=(1–3)×10⁻³ in Z110 freshly formed cosmic-rays (time interval 10³–10⁷ years).The method proposed can provide the necessary and sufficient conditions for the discovery of Z110 nuclei in nature.     

On search and identification of relatively short-lived superheavy nuclei (<Emphasis Type="Italic">Z</Emphasis> ≥ 110) by fossil track studies of meteoritic and lunar olivine crystals

The main goal of the present work is the search for and identification of relatively stable nuclei of superheavy elements (SHE) (Z>110) in galactic matter by fossil track study of nonconducting crystals from the surface of meteorites and rocks from the lunar regolith. Nuclei of SHE are thought to be the products of nucleosynthesis in explosive processes in our Galaxy (supernova r-process nucleosynthesis and, especially, neutron-star formation, etc.). When accelerated to relativistic energies in the Galaxy, they can produce extended trails of damage in nonconducting extraterrestrial crystals. The lifetime of such SHE in galactic cosmic rays will range from 10³ to 10⁷ yr to be registered in extraterrestrial crystals. To search for and to identify the superheavy nuclei in the galactic cosmic rays, it was proposed to use the ability of nonconducting extraterrestrial crystals such as olivines, pyroxenes, and feldspars to detect and to store for many millions of years the trails of damage produced by fast Z≥23 nuclei coming to rest in the crystalline lattice. The track lengths of fast Z≥23 nuclei are directly proportional to Z² of these nuclei. The nuclei of SHE produce, when coming to rest in a crystal volume, tracks that are a factor of 1.6–1.8 longer than the tracks due to cosmic-ray Th and U nuclei. To identify the tracks due to superheavy nuclei, calibrations of the same crystals were performed with accelerated Au, Pb, and U nuclei. For visualization of these tracks inside the crystal volume, proper controlled annealing and chemical etching procedures were developed. Since 1980, fossil tracks due to Th and U nuclei have observed and unambiguously identified (1988) by subsequent calibrations of the olivine crystals with accelerated U, Au, and Pb ions. The number of tracks of Th and U nuclei measured in olivine crystals totaled more than 1600, as compared with the prior 30 events. The other approach to identifying SHE in nature is to search for tracks in phosphate crystals from spontaneous fission of Z ≥ 110 nuclei; these produce two-prong and three-prong fission fragment tracks and differ significantly from the tracks from spontaneous fission of ²³⁸U and ²⁴⁴Pu nuclei. Extraterrestrial phosphate crystals of lunar and meteoritic origin will be investigated. Such SHE nuclei can survive in crystals of extraterrestrial rocks and produce spontaneous fission tracks, if the lifetime is more than 5×10⁷ yr.     

Track recording properties of soda glass detector for accelerated heavy ions

The etch pit diameters of soda glass detector samples exposed to ₅₄ ¹³² Xe-ions of different energies are measured for different etching times after etching the detector in a ‘new etchant’ free of the adverse effect of the etch product layer. The dependence of track diameter on the energy and on the energy loss, dE/dx of ₅₄ ¹³² Xe-ion in soda glass has been presented. The energy resolution of soda glass and the critical angle for etching of fission fragment tracks in glass detectors have also been determined. The maximum etched track length of ₅₄ ¹³² Xe-ion in soda glass has been compared with the theoretical range. The effects of different annealing conditions on bulk etch rate of glass detector and on diameters of ₅₄ ¹³² Xe-ion tracks have been presented. Experimental results show that there is a decrease in track etch rate, etching efficiency and etchable range of ₅₄ ¹³² Xe-ions with annealing. The annealing of oblique tracks shows that the vertical tracks are more stable than the oblique tracks.     

Detection of energetic light charged particles by solid state nuclear track detectors

Experiments have been carried out to detect ₂ ³He particles and : rotons having energies up to 10 MeV/nucleon by using Kodak CA80-15, cellulose nitrate plastic track detector. Various etching conditions were tried in order to develop tracks for whole of the energy range considered. Detailed analysis seems to indicate that at high energies, the tracks are mainly produced by “secondaries” (elastically scattered nuclei of C, N, O and H, and other reaction products) while in the low energy region, the slowed down “primaries” play the dominant role. The prolonged etching factors of these detectors for different types of tracks have also been obtained and used to derive their average etchable ranges in the materials concerned.     

Neutron response study using poly allyl diglycol carbonate

The results of an experimental work aimed at improving the performance of the CR-39 nuclear track detector for neutron dosimetry applications are reported. A set of CR-39 plastic detectors was exposed to ²⁵²Cf neutron source, which has the emission rate of 0.68 × 10⁸ s⁻¹, and neutron dose equivalent rate 1 m apart from the source is equal to 3.8 mrem/h. The detection of fast neutrons performed with CR-39 detector foils, subsequent chemical etching and evaluation of the etched tracks by an automatic track counting system was studied. It is found that the track density increases with the increase of neutron dose and etching time. The track density in the detector is directly proportional to the neutron fluence producing the recoil tracks, provided the track density is in the countable range. This fact plays an important role in determining the equivalent dose in the field of neutron dosimetry. These results are compared with previous work. It is found that our results are in good agreement with their investigations.      

Study of fossil tracks due to 50 < or = Z < or = 92 galactic cosmic ray nuclei in meteoritic crystals: results and perspectives

A new approach to the problem of investigation of charge and energy spectra of ultra heavy Galactic cosmic ray nuclei, based on fossil track study of extraterrestrial olivine crystals has been developed. The results of an investigation of ultra heavy Galactic cosmic ray nuclei (Z=50-92) in meteoritic olivine crystals are presented. The technique was based on calibration of olivine crystals with accelerated Xe, Au, Pb and U ions and well-controlled partial annealing of "fresh" and "fossil" tracks. It allows us to determine the charge spectra and abundances of cosmic ray nuclei based on fossil track length study in meteoritic and Moon crystals. The comparative studies of the spectra of "fossil' tracks and tracks due to 208Pb and 238U nuclei have shown that the group of 210 micrometers "fossil" tracks, first observed in 1980 at JINR is due to Th-U nuclei-products of recent r-process nucleosynthesis in our Galaxy. The method in principle allows one to resolve Pt-Pb peaks in fossil tracks, to establish the upper limit of the abundance of Z>110 nuclei in the Galactic cosmic rays at the level < or = 10(-3) to the abundance of actinide nuclei and to get information on the history of Z>50 cosmic ray nuclei in time interval up to 220 M.Y.     

Tracks of 18·56 MeV/u 40Ar ions in Lexan polycarbonate detector

Latent damage tracks of energetic⁴⁰Ar ions (18·56 MeV/u) have been recorded in Lexan polycarbonate detector. Bulk and track-etch parameters are evaluated under successive chemical etching. Our results show a linear correlation between the measured track-etch rate along the track and the corresponding total energy-loss rate and predict a threshold value of 5·0 MeV mg⁻¹ cm² for track registration. Maximum etchable track lengths of⁴⁰Ar ions as a function of energies have also been measured and compared with three different sets of theoretical ranges.     

Annealing of 54 132 Xe-ion tracks in Lexan and Makrofol plastic track detectors

Samples of Lexan and Makrofol-E polycarbonate plastic track detectors were exposed to 1·1 MeV/N ₅₄ ¹³² Xe-ions to investigate the thermal track fading properties of these plastics. The experimental results show that there is no effect of annealing on the bulk etch rate while the track etch rate decreases with annealing. The track diameter decreases with increase in annealing time and temperature. It is also observed that the track density is reduced as a result of annealing. The experiments reveal that the track lengths are, in general, decreased by the application of heat and that the oblique tracks are less stable than the vertical tracks. The decrease in diameter of ₅₄ ¹³² Xe-ion tracks in Makrofol-E due to heat treatment is faster than that of ₅₄ ¹³² Xe-ion tracks in Lexan.     

Study of fossil tracks due to VH and VVH groups of cosmic ray nuclei in olivine crystals from Luna-16 and Luna-24

The olivine crystals from lunar regolith samples taken by the Soviet unmanned spacecrafts Luna-16 and Luna-24 were investigated. Eleven 0.5 –1.0 mm size olivine crystals were mounted in epoxy, polished and then etched in modified WO₄ solution. The Fe-group track densities up to 10⁸ tracks.cm⁻² (Fe-group) were measured under optical microscope. The tracks of length greater than 30 microns due to Z ≥ 36 cosmic ray nuclei are counted for VVH tracks density for all the crystals. The VVH / VH track densities ratio for these lunar olivine crystals varies from 1.25×10⁻⁴ to 2×10⁻³. It corresponds to the averaged depth of these crystals in lunar soil of 2–8 cm during galactic cosmic ray exposure. Lunar crystals are well suited for VVH track studies due to a very high track density. Two crystals were annealed at 430°C for 32 hrs. This procedure eliminates iron group tracks completely and leaves etchable tracks of nuclei with Z 50 even in the olivine crystals with Fe-group tracks up to 1–2×10⁸ tracks cm⁻². We were able to measure two tracks with the length 195 and 210μm which were produced by Th---U group of Galactic cosmic ray nuclei.     

Recrystallization of amorphous nanotracks and uniform layers generated by swift-ion-beam irradiation in lithium niobate

The thermal annealing of amorphous tracks of nanometer-size diameter generated in lithium niobate (LiNbO₃) by Bromine ions at 45 MeV, i.e., in the electronic stopping regime, has been investigated by RBS/C spectrometry in the temperature range from 250°C to 350°C. Relatively low fluences have been used (<10¹² cm⁻²) to produce isolated tracks. However, the possible effect of track overlapping has been investigated by varying the fluence between 3×10¹¹ cm⁻² and 10¹² cm⁻². The annealing process follows a two-step kinetics. In a first stage (I) the track radius decreases linearly with the annealing time. It obeys an Arrhenius-type dependence on annealing temperature with activation energy around 1.5 eV. The second stage (II) operates after the track radius has decreased down to around 2.5 nm and shows a much lower radial velocity. The data for stage I appear consistent with a solid-phase epitaxial process that yields a constant recrystallization rate at the amorphous-crystalline boundary. HRTEM has been used to monitor the existence and the size of the annealed isolated tracks in the second stage. On the other hand, the thermal annealing of homogeneous (buried) amorphous layers has been investigated within the same temperature range, on samples irradiated with Fluorine at 20 MeV and fluences of ∼10¹⁴ cm⁻². Optical techniques are very suitable for this case and have been used to monitor the recrystallization of the layers. The annealing process induces a displacement of the crystalline-amorphous boundary that is also linear with annealing time, and the recrystallization rates are consistent with those measured for tracks. The comparison of these data with those previously obtained for the heavily damaged (amorphous) layers produced by elastic nuclear collisions is summarily discussed.     

Electrolytes in etching of latent tracks of heavy ions in polyethylene terephthalate

Previously unknown features of etching of polyethylene terephthalate, latent tracks of multiply charged accelerated ions in it, and track membrane pore formation are considered. It was found that K ions (in the form of KCl salt) in a KOH solution enhance etching of both initial polyethylene terephthalate and tracks. Ba²⁺ ions enhancing etching of initial polymer significantly inhibit etching of tracks. It is assumed that etching inhibition is associated with Ba²⁺ ion adsorption on track active centers. The features detected are used to fabricate track membranes with thin selective layer.     

Use of the temperature peak model for the description of track formation in semiconductor crystals irradiated by fast heavy ions

An attempt to apply the temperature peak model to describe the formation of defects and tracks in semiconductor crystals is made for the first time. The temperature dependences of model parameters, such as specific heat, thermal conductivity, and electron-phonon coupling coefficient are obtained. Agreement between the theoretical results and experimental data for InP and Ge crystals irradiated by ultrafast heavy ions indicates the adequacy of the model, with which one can evaluate the temperature of the local area near the ion trajectory, as well as the diameters of the molten region and experimentally observed track region. The diameter of the cylindrical molten region that forms along the path of 250-MeV Xe⁺ ions in InP is predicted to be 20 nm, and the measured cross-sectional diameters of the tracks fall into the range 7–15 nm.     

Conductivity of aged non-overlapping and overlapping tracks in ion irradiated polyimide

Non-overlapping as well as overlapping tracks of energetic ions have been introduced into polyimide foils. After aging their conductivity was measured. This — to our knowledge — first systematic study shows that conductivity does not only result from multiple track overlapping, but can be found already in single ion tracks. This conductivity is shown to be primarily a consequence of electronic energy transfer. The conductivity of single ion tracks is higher than that of typical insulators, but still orders of magnitude lower than that of typical semiconductors. The conductivity is independent of the applied electric field strength until at excessive voltages the electric current increases nonlinearly up to complete breakthrough. The total conductivity of an irradiated polyimide foil increases proportionally with ion fluence for large ion track spacings, and approaches saturation when the electronically active track regimes begin to overlap. Above some thousand times track overlapping however, new chemical and structural changes in the irradiated material lead to another strong increase in conductivity.     

The chemical etching of fission fragment tracks in natural fluorite

An experimental study of the mechanism for chemical etching of fission fragment tracks in the natural mineral fluorite is described. A systematic search showed that a 3:1 mixture by volume of sulphuric to hydrochloric acids was a most appropriate etchant. Experiments directed at determining the etching efficiency as a function of solvent temperature are also discussed. The preferential track etch ratioVt/Vg, the track length and the track density all depend upon the time and temperature of annealing.

It is variations of the fission track density in fluorite, with etching time and annealing temperature, which make possible an overall geophysical interpretation of annealing data for the mineral in terms of the paleoisotherm of its intrinsic fission track clock.

An interactive image analysis system INTIMAN, assembled for the swift and automatic readout of fission fragment track measurements, in both crystalline and non-crystalline materials, is described. Normal procedures for measuring and analyzing tracks are outlined.     

A new method for detection of alpha particles in 1 mm thick polycarbonate detectors using 50 Hz – HV ECE method

Recent studies in our laboratory have proved that electrochemical etching (ECE) of polycarbonate track detectors (PCTD) under 50 Hz – high voltage (HV) field conditions has potentials for time-integrated heavy charged particle detection and dosimetry applications. The rationale in the study is the ECE process of alpha particle tracks in 1 mm thick PCTDs by a 50 Hz – HV generator at optimized ECE conditions. Tracks of 3.2 MeV alpha particles from a collimated beam of an ²⁴¹Am source degraded in air and background tracks were registered. The effects of HV and ECE duration on alpha track registration efficiency and track diameters were studied for 3 sets of 50 Hz – 4, 5 and 6 kV field conditions in a PEW solution (potassium hydroxide, ethanol and water) at 26 °C. The optimized ECE conditions obtained at this stage of development for 1 mm thick PCTDs are 50 Hz – 4 kV in PEW solution at 26 °C for 10 h. Alpha track registration efficiency at 3.2 MeV is about 30% with 37 ± 6 μm mean track diameter. The mean background track density at the above stated optimized conditions is about 571 ± 16 tracks.cm⁻² with a mean diameter of 65 ± 5 μm. All tracks are observable by the unaided eyes. The mean background track diameter is near two times larger than that of alpha particle tracks at the optimum conditions applied; they are easily distinguished against each other. This high background track density while at this stage of development seems a drawback for low dose and low fluence particle applications, it has minimal effects on high fluence ion detection applications. The simple 50 Hz – HV generator used proved to be convenient for efficient alpha track amplifications. Studies are underway for improvement of the method in particular for reducing background track density.     

Different shapes of tracks in phlogopite, biotite and soda lime glass

Etched track opening geometries in Biotite, Phlogopite and soda-lime glass irradiated with swift heavy ions [¹⁹⁷Au(11.64 MeV/n), ¹³⁶Xe(11.56 MeV/n), ⁵⁸Ni(11.56 MeV/n)] at different angle of incidence have been studied using appropriate chemical etching technique. Different geometries (Hexagonal, irregular polygon, triangular in case of Biotite and Phlogopite, and circular & elliptical in case of soda lime glass detector) of heavy ion tracks are reported in the present investigations using optical microscope. The different shapes of these heavy ions track geometries are found to be related with various target-projectile parameters (viz: type of projectiles, energy, stopping power, angle of incidence of the projectile, density of defects and its reactivity with etchant, etching conditions and chemical structure of the detectors). The dependence of different shapes of heavy ion tracks in isotropic and anisotropic medium on the variation of radiation damage densities along the ion trajectories have also been discussed in the present paper.      

High Energy Charged Particle Registration in CR-39 Polycarbonated Detector

Track etch rate characteristics of CR-39 plastic detector exposed to ²⁸Si ions of 670 MeV energy have been investigated. Experimental results were obtained in terms of frequency distribution of the track diameter, track density and bulk etching rate. A dependence of the mean track diameter on energy was found. The application of the radiation effect of heavy ions on CR-39 in the field of radiation detection and dosimetry are discussed. Results indicated that it is possible to produce etchable tracks of ²⁸Si in this energy range in CR-39. We also report the etching characteristics of these tracks in the CR-39 detector.     

The influence of etching parameters on the sensitivity of plastics

Abstract

It seems that the critical rate of primary ionization for track registration must also depend on the etching conditions. Simple experimental methods are presented to show a possible change in registration sensitivity as a function of the chemical parameters. It was proved, from investigations of α-particle tracks, that the sensitivity of a cellulose acetate detector can considerably depend on the concentration and type of etching reagent. Quantitative data are given on the ratio of the rate of chemical etching along the track and on the detector surface as a function of concentration of NaOH solution for tracks of fission fragments registered in plastics of cellulose acetate, polycarbonate and polyethylene-terephthalate.     

Observations of fission-tracks in zircons by atomic force microscope

The fission-track (FT) method is a dating technique based on the observation of damage (tracks) by spontaneous fission of ²³⁸U left in a mineral. The date is calculated from the track density and the uranium concentration in the mineral. This is possible because the number of tracks is a function of uranium concentration and time since the start of track accumulation. Usually, the number of tracks is counted under an optical microscope after etching (chemical expansion of a track). However, as FT density per unit area rises, it becomes difficult to count the number of tracks. This is due to the fact that FTs overlap one another and are unable to be readily distinguished. This research examines the potential of atomic force microscope (AFM) for FT dating using zircons, which are likely to show higher FT density than other minerals due to their high U concentrations.To obtain an AFM image for a sample prepared for FT dating, removing the static electricity of the sample is essential to avoid an unexpected movement of the cantilever. A grain should be wider than about 30 μm to bring the cantilever on the mineral surface. Polishing with a fine grained compound is very important. There is not much difference in sharpness between images by AC mode (scanning with vibrating cantilever at a constant cycle) and Contact mode (scanning with the cantilever always in close contact with the surface). To confirm how tracks can be identified with the AFM, an AFM image was compared with an image obtained with the optical microscope. When change in the number of tracks and their shapes were observed through stepwise etching, the track expanded as the etching time increased. In addition, the etching rate was slower for large tracks than those for small tracks. This implied that the AFM can be used to observe etching of zircons with different degrees of nuclear fission damage. A track that could not be seen with the optical microscope due to insufficient etching could be observed by AFM methods, indicating the possibility of FT dating with high track densities using AFM after relatively short etching periods.