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.     

Man-made plutonium in environment — possible serious hazard for living species

It is pointed out that, contrary to the situation with natural Rn, the growing concentration of man-made Pu in environment — natural water soil plants and food — can provide the serious danger for all kind of animals and especially for mankind. Really, as it was established recently, element Pu is accumulated in human body during all the life and the dangerous concentration estimated to be 10⁻¹² – 10⁻¹³ grapm Pu per gram of human tissues. Unfortunately up to now there are no simple nonexpensive methods of Pu determination at the level of sensitivity 10⁻¹⁴ – 10¹⁵ g/g which can provide the determination of Pu even in 0.2 g of human tissue. We warn that now the average concentration of Pu in human body is not less than 10⁻¹⁴ g/g and much higher for some “hot” regions in Europe and Asia. We propose to discuss the problem of organizing world net exploration of Pu in environment — similarly to Rn exploration program — and personnel Pu monitoring for inhibitions of Pu damaged regions. Our approach to the problem is based on chemical separation of Pu, on determination of Plutonium by high fission cross section with thermal neutrons ²³⁹Pu(n,f) reaction and by control of possible admixture of ²³⁵U isotope by ²³⁸U(γ, f) reaction in Pu preparations. The problem of increasing of sensitivity of Pu analysis up to 10⁻¹⁴ – 10⁻¹⁵ g/g is discussed in detail.     

Cosmic history of the Bragin pallasite: evidence from the fission-track analysis

Chronology is rather a weak point in the investigation of pallasites, the stony-iron meteorites. No chronological data are known for the Bragin pallasite. Our attempt to reconstruct its cosmic history was based on the interpretation of fission-track analysis data. To apply this method only uranium-rich phosphates can be used. Extremely rare grains of stanfieldite were extracted from the silicate sawing residue and from the pallasite sample directly.

The researches pursued by us made it possible to find two populations of fossil tracks in stanfieldite grains. The tracks of these populations strongly differed both in size, shape and character of distribution. The first population, consisting of short (L2–6 μm instead of L8–12 μm for induced fission tracks), round-shaped tracks irregularly distributed, as we suppose, suffered an intense heating process, which caused a significant amount of partial annealing. The second population, consisting of longer (L8–12 μm), rhombic-shaped tracks homogeneously distributed, occurred after this thermal event. Only the second population track density was used for the fission-track age calculation.

After correction of the fossil track density, consisting of the second population tracks, for other possible track sources, the revealed tracks were unequivocally identified as those due to the spontaneous fission of ²⁴⁴Pu and ²³⁸U. The largest part of them was attributed to the spontaneous fission of ²⁴⁴Pu; ρ_Pu/ρ_U≈3. The model fission-track age of the studied pallasite turned out to be 4.20 Gyr. This value fix the time of the last shock/thermal event in the cosmic history of the Bragin pallasite, which had caused the partial annealing of tracks presented to that time and “fission-track clock” reset.     

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.     

Some contributions from SSNTD towards nuclear science: from multifragmentation towards accelerator driven systems (ADS)

Three examples are chosen to show the importance of SSNTD as one of the essential tools in nuclear science:

(1) Multifragmentation into more than two heavy reaction products: Starting with the observation of three heavy reaction products in the interaction of relativistic protons or 414 MeV ⁴⁰Ar with actinides in the early 1960s, up to the observation of five heavy reaction products in the interaction of 2400 MeV ²³⁸U with uranium, SSNTD had a leading role in this research.

(2) In the search for superheavy elements (SHE: Z around 114): Many different techniques are used. However, SSNTD are exclusively decisive in the possible observation of SHE within the heavy element component of galactic cosmic rays.

(3) Accelerator driven systems: They are increasingly important in the discussion of energy producing nuclear power stations and in the corresponding ability to transmute long-lived poisonous radioactive materials (above all plutonium) into shorter lived fission fragments or stable nuclides. SSNTDs play an important role in the determination of the energy dependent neutron fluence in small volumes (≈cm³) or in the exact beam profile determinations of the primary proton beams.

This contribution ends with an outlook into possible future fields of physics research: With the advent of a new generation of relativistic heavy ion accelerators, such as the NUCLOTRON at the JINR in Dubna, Russia, and RHIC in Brookhaven in the United States, one can continue to study (and finally confirm or disprove) all phenomena mentioned already, as well as additional controversial phenomena, such as “enhanced nuclear cross-sections over short distances”, called colloquially “anomalons”. Again SSNDT can be used in at least a twofold manner as an important tool: (a) the enhanced neutron production with ¹²C ions or heavier ions in thick targets at energies above approximately 50 GeV and (b) the reduced “mean-free-path” of secondary fragments produced by the same heavy and energetic ions.     

Importance of the photo-beta process for the synthesis of “p” elements in stellar conditions

In this work, we compare positon capture and photo-beta disintegration probabilities in several stellar conditions.

We show that the second process can be neglected with regard to the first one in strongly endothermic nuclear transitions, whereas photo-beta disintegration can be competitive with positon capture and even can have a greater likelihood than the latter process in weakly endothermic and exothermic transitions.

In the range of temperature we consider here (T ≈ 10⁹ °K), it appears that the lifetime ratio τ(ph)/τ(e_c⁺) against photo-beta disintegration and positon capture is the smallest for densities in the neighbourhood of 10⁶ g/cm³.

Thus, we arrive at the conclusion that the photo-beta process can play a role in the synthesis of two “p” elements at least, ₆₂¹⁴⁴Sm and ₈₀¹⁹⁶Hg, for which the ratios τ(ph)/τ(e_c⁺) are close to 10 and 20, respectively, in the most favourable stellar conditions.     

Influence of intensive γ and electron radiation on tracks formation in the PM-355 detectors

Solid-state nuclear track detectors have found wide use in various domains of science and technology, e.g. in plasma experiments. The track detectors used in the fusion-oriented experiments encounter “harsh” conditions (intense X-ray and neutron radiation, heat impact, shock waves and plasma fluxes). Therefore, such detectors should be tested under similar conditions. This paper concerns influence of electron and γ radiation on the track formation in PM-355 detectors. Samples were irradiated with 1.5-MeV protons and ⁴He-ions, and with 5.5 MeV particles. After that they were exposed to γ and electron radiation. Irradiation doses were varied from 100 kGy up to 2000 kGy. The etching was performed in steps, and a bulk etching rate (V_B) was determined versus an absorbed dose of electron and gamma radiation.     

Dynamics of antiproton cooling in a positron plasma during antihydrogen formation

We demonstrate cooling of 10⁴ antiprotons in a dense, cold plasma of 10⁸ positrons, confined in a nested cylindrical Penning trap at about 15 K. The time evolution of the cooling process has been studied in detail, and several distinct types of behavior identified. We propose explanations for these observations and discuss the consequences for antihydrogen production. We contrast these results with observations of interactions between antiprotons and “hot” positrons at about 3000 K, where antihydrogen production is strongly suppressed.     

Experimental study of radioactive aerosols in the vicinity of the Chernobyl Nuclear Power Plant

Study of radioactive aerosols in the relocation zone and in the populated areas have been carried out for a number of years. The experiments on modelling resuspension were performed while conducting agricultural work. Nuclear track radiography and alpha spectrometry with radiochemical extraction of plutonium were used as analytical methods for the determination of the transuranium elements contents. The distributions of radioactive particles were obtained as to activity and sizes. Specific activity of “hot particles” increases with decreasing diameter. In aerosols selected at a distance of more than 10 km from the Chernobyl NPP pure fuel particles with sizes of more than 5 μm were not found. The activity of the finely dispersed fraction of aerosols, which is more dangerous when inhaled by the organism, is comparable with a total activity of large particles.     

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.     

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.     

Automation system for optical counting of nuclear tracks

An automation system consisting of the microscope, video camera and Pentium PC with frame recorder was created. The system provides counting of nuclear tracks on the SSNTD surface with a resolution of 752 × 582 points, determination of the surface area and main axis of the track. The pattern recognition program was developed for operation in Windows 3.1 (or higher) ensuring a convenient interface with the user. In a comparison of the results on automatic track counting with the more accurate hand mode it was shown that the program enables the tracks to be detected even on images with a rather high noise level. It ensures a high accuracy of track counting being comparable with the accuracy of manual counting for densities of tracks in the range of up to 2·10⁵ tracks/cm². The automatic system was applied in the experimental investigation of uranium and transuranium elements.     

Evaluation of the screening correction to allowed β-decay for light elements

The screening correction to allowed β-decay is given to order ³ and is compared with the “exact” value for light elements.     

Hollow particle tracks in AgCI-detectors

In selected Cd-doped monocristalline silverchloride detectors we observe developed tracks from particles at LET values > 300 keV/μm AgCl and charge state values > 9, without a visible central region: the “hollow track”. The microdensitometric lateral profile shows a density decrease near the track axis, up to a radial extension of some microns from highly charged particles as Fe or U-ions of several MeV/u; the tracks of fast U- or Fe-projectiles, moreover, represent an entanglement of delta-electron tracks only. A recent reanalysis of this “hollow track”-effect is suggested to be caused by recombination effects and structural distortions. They occure in areas of high delta-electron density; together with the characteristic process of track formation in crystalline AgCl/Cd they enable us to vizualise and to measure the radial range of distortion and to evaluate the threshold of the energy density above which the destruction occurs.     

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.     

Escape of charged particles at stopping annihilation of antiprotons in the heavy nuclei of nuclear photoemulsion

“Rare” annihilation channels for antiprotons stopping on heavy (Ag, Br) nuclei of photoemulsion, have been sought; 4872 stops of antiprotons on photoemulsion nuclei are analysed. Events of formation and decay of the hyperfragment _Λ⁴H, escape of ⁸He and ⁸Li nuclei, one-prong stars with the mean range 79.5±5.1 μm of secondary slow “b” particles are found among the annihilation stars at capture on nuclei (Ag, Br). The lower limits for the production probability of _Λ⁴H and ⁸He, ⁸Li nuclei per antiproton stopping in the nuclei (Ag, Br) are

W_Λ⁴H2×10⁻⁴ and W_⁸He,⁸Li=(1.3±0.6)×10⁻³.

The branching ratio for the production of one-prong stars with the secondary “b” particles is at least (1.3±0.6)×10⁻³. Possible mechanisms for a production of these events in annihilation processes are considered.     

Methods of high-sensitive analysis of actinides in liquid radioactive waste

A set of methods has been developed to determine actinides in liquid radioactive waste for solving the problems of radiation, nuclear and ecological safety of nuclear reactors. The main method is based on the radiochemical separation of U, Np–Pu, Am–Cm on ion-exchange and extraction columns. An identification of radionuclides and determination of their content are performed using alpha-spectrometry. The microconcentrations of the sum of the main fissile materials ²³⁵U and ²³⁹Pu are determined with plastic track detectors. An independent method of ²³⁸U content determination is the neutron activation analysis. ²⁴¹Am content is possible to be determined by gamma-spectrometry. A chemical composition of macrocomponents is determined by the atomic-absorption spectrophotometry method.     

Nuclear tracks in solids: registration physics and the compound spike

Observations of GeV heavy ion and MeV cluster-ion tracks in crystalline solids give us new insight into registration physics. Thermal and ion explosion spikes no longer compete; a ‘compound spike’ accounts for both. Ion explosion dominates for surface tracks (electronic sputtering). And there can also be transient plasma stopping in the bulk. For clusters there are ‘vicinage effects’—both electronic and nuclear—which can influence track dimensions and structure. Displacement cascades in large energetic clusters may lead to projectile “fission” and coherent flow into sub-tracks. The absence of tracks in certain targets, and their size/structure in others, leads to a model of projectile assisted prompt anneal (PAPA) in 10⁻¹¹s, either partial or complete, often by swift epitaxy, on elemental lattices (e.g. silicon) or on compound sublattices (e.g. fluorite). Phase transformations are important, but simple target amorphization is rare—the exception, not the rule. For many targets the thermal spike (macroscopic) fails, since ‘point’ defects (atomistic) characteristic of the target, their motion, and the electronic band structure, determine latent track detail. Circumstances in which the Bragg Rule of Additivity fails completely are revealed, and the kinetic threshold for constructive phase transitions in tracks described. This same track physics applies generally also to geothermometry—the opposite time extremum (10⁺¹¹s)—where annealing is due to defect assisted delayed anneal (DADA). Differences between etching rates of induced and spontaneous fission tracks can be explained. The geothermobarometric “Wendt/Vidal effect” (2002)—combined pressure, temperature and stress (with time) influences on fission track annealing (in e.g. apatite)—is briefly discussed.     

Gd, U, Pu and Cm alpha particle energy analysis using tracks in solids

This paper presents advances in a procedure for alpha particle analysis using the nuclear tracks formed in solid-state materials. This method is based on the relationship between the energy deposited in the material by ionizing particles and the track developed after a well-established chemical process. The experimental study included alpha particles in the energy range from 3.2 to 5.8 MeV emitted by ¹⁴⁸Gd, ²³⁸U, ²³⁹Pu and ²⁴⁴Cm. The quantitative results provide a clear signature to identify each one of the radioisotopes based on the formed track parameters. The track analysis is performed with a digital image analysis system associated with a PC mathematical processor. The wide range energy response makes this method a promising analysis system.     

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.