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.     

Studies on the track formation mechanism of the heavy ions in CR-39

The bulk etch rate for two types of CR-39 detector was measured as a function of temperature and the activation energies of bulk etching was determined. Experimental values of track etch rate were derived directly from the function of the succesive measured track length vrs. etching time for ²⁰⁹Bi, ¹²⁹Xe and ²⁰Ne ions.

The maximum etchable length of 13 MeV/u ²⁰⁹Bi and 13.04 MeV/u ¹²⁹Xe ions have been measured at and below these energies. A comparison of the measured and calculated track length data is presented.     

Cosmic history of some pallasites based on fossil track studies

Investigation of fossil charged-particle tracks in various mineral phases of extraterrestrial samples is a powerful method for research the early stages of the solar system. Examination of fossil charged-particle tracks in the phosphate and olivine crystals of 5 pallasites coupled with U content determination allowed the estimation of the contributions of all possible track sources to the total track density and calculation of a value of model fission-track age.

Phosphate crystals from all studied pallasites were established to contain fossil tracks due to galactic cosmic rays (VH, VVH nuclei); induced fission of U and Th by cosmic rays; spontaneous fission of ²³⁸U; spontaneous fission of extinct short-lived ²⁴⁴Pu nuclei presented in significant quantities in the early solar system. The discovery of a high track density attributed to the extinct ²⁴⁴Pu pointed obviously to the high value of the fission-track age. Model fission-track ages of (4.37±0.02) Gyr for the Marjalahti pallasite; (4.37±0.01) Gyr for the Omolon pallasite; (4.19±0.02) Gyr for the Bragin pallasite; (4.18±0.03) Gyr for the Krasnoyarsk pallasite; (4.21±0.02) Gyr for the Brenham pallasite were calculated. The comparison of represented data with petrographic analyses allowed us to interpret a value of fission-track age as the time of the last intensive shock/thermal event in the cosmic history of a pallasite.     

Energy loss dependent transversal etching rates of heavy ion tracks in plastic

By the method of electrolytical etching track etching rates V_t and corresponding transversal track etching rates V_trans of single heavy ion tracks in thin Makrofol KG foils have been measured at ion energies from 10–480 MeV/u. Makrofol KG foils of 8 μm thickness were irradiated perpendicular to the surface with ⁷⁹Au and ⁵⁴Xe ions at specific energies with energy loss values of REL=(10–90) ^*10³ MeVcm²/g at GSI Darmstadt, Germany, and Lawrence Berkeley Lab., Cal., USA. Using the electrolytical etching method by measuring the resistance of the foil during the etching process (etching conditions: 6n NaOH, room temperature and controlled 50° C) the breakthrough time and track etching rates V_t, V_trans and V_m (bulk etching rate) were analysed. Response curves (V_t/V_m)-1 as a function of Restricted Energy Loss (REL), the maximum extension of the ion induced damage perpendicular to the ion path and the dimension of the ion track core depending on the deposited energy can be estimated.     

Fossil track studies of the Omolon pallasite crystals

The olivine and stanfildite crystals from Omolon pallasite meteorite were selected from some residue and from locations of an about 150 g fragment of that meteorite in the Meteoritic Committee, Moscow, Russia. The radiation age of Amnion pallasite was determined to be about 78 MY The Olivine crystals were mounted in epoxy resin, polished and etched in Krishnaswami solution, modified by adding 30 g per liter oxalic acid. The etching of the olivine crystals was performed in hermetically closed vessels during 36–72 hours at T = 100 ° C. The measured Fe- group track density varies from 3 × 10⁴ up to 2.6 × 10⁵ track. cm⁻². The measure in 12 Fe-group track rich olivine 43 track due to VVH nuclei were found. It means that the depth of ablation of Omolon meteorite does not exceed (8.2 ± 2.1) cm out of preatmospheric surface for the most favourable locations.     

Fission-track analysis of meteorites: Dating of the Marjalahti pallasite

The results of the Marjalahti pallasite fission-track age determination are presented. Thorough examination of fossil tracks in the phosphate (whitlockite) crystals coupled with U-content determination in whitlockites can make it possible to estimate the contributions of all possible track sources to the total track density and to calculate a model fission-track age.

It is found that whitlockite crystals of the Marjalahti pallasite contain fossil tracks due to galactic cosmic rays (VH, VVH nuclei); fission of U and Th induced by cosmic rays; spontaneous fission of ²³⁸U; and spontaneous fission of extinct, short-lived ²⁴⁴Pu present in significant quantities in the early solar system.

A great track density attributed to the extinct ²⁴⁴Pu testifies to the high fission-track age. The model fission-track ages of (4.31±0.02)×10⁹ yr for the Marjalahti pallasite are calculated. Petrographic studies allow us to interpret the fission-track age as the time of the last shock/thermal event in the cosmic history of the pallasite.     

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.     

Technique for determining the charge of cosmic ray nuclei by tracks in olivine crystals from meteorites

A technique for identifying the charge of cosmic ray nuclei, based on measurements of the length and average etch rate of tracks chemically etched in olivine crystals from the Marjalahti pallasite is described.     

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.     

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.     

Submicroscopic analysis of tracks in mica

Tracks of 49 MeV ³⁵Cl ions in muscovite mica were analyzed by transmission electron microscopy up to 10 Å resolution applying the track replica method. The enlargement of the track diameter is measured as a function of etching time. The track shape evolution shows circular tracks for very short etching times. By increasing the etching time the tracks gradually become ovals. For longer etching times, tracks show the characteristic rhombic shape of the bulk region. A non monotonous decrease of the track velocity vs. radius is reported. Formation of a low velocity shell in the intermediate region between the central amorphous zone and the non-perturbed crystalline lattice is suggested.     

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.     

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.     

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.     

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.     

Low energy alpha particle spectroscopy using CR-39 detector

The possibility of using CR-39 to measure the depth profile of ¹⁰B in Si is analysed. The measuring technique exploits the ¹⁰B(n, )⁷Li nuclear reaction. For this reason the track parameters (size, optical properties) of low energy alpha-particles (<1.47 MeV) were studied. The results showed that an energy resolution of about 100 keV could be obtained by an appropriate selection of etching conditions. The profile of ¹⁰B in Si at a depth as small as 1 μm can be measured.     

Detecting galactic cosmic ray transuranium nuclei in olivine crystals from meteorites

Results from the experimental search for and identification of tracks from the superheavy and transuranium nuclei of galactic cosmic rays in pallacite olivine crystals, conducted as part of project OLIMPIA [1], are presented. To date, 170 crystals from Marjalahti and Eagle Station pallacites have been processed and 6800 tracks corresponding to nuclei with charges Z > 55 have been found; 45 of these are from nuclei with charges of 88 < Z < 92 and three super-long ones were produced by nuclei with Z > 105. The charge of one of these nuclei is estimated in the first approximation as Z = 119(+10,?6). Our data confirm the hypothesis of islands of stability for natural trans-Fermi nuclei.     

Damage morphology of Kr ion tracks in apatite: dependence on dE/dX

With the aim of characterizing damage along nuclear tracks in apatite, Durango fluoroapatite monocrystals were irradiated under a high fluence ⁸⁶Kr ion beam at the G.A.N.I.L. (Grand Accélérateur National d'Ions Lourds, Caen, France). The resulting irradiation damage was studied by associating CRBS spectrometry and chemical etching. By applying Poisson's law to the backscattering results, the nuclear track average effective radius R_e was calculated for different steps along the ion path. On the other hand, the chemical etching experiments allowed us to deduce three different damaging morphologies in correspondence to the R_e values. For the first time in apatite, it has been shown that a defect fragmentation produced along the ion paths may be detected by chemical etching. These results were also applied to fission tracks in order to quantify the damage rate and to describe the damage morphology evolution along fission fragment paths.     

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.