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.     

Comparison of monthly and daily isotopic composition of precipitation in the coastal area of Slovenia

The stable isotopic composition (delta(2)H and delta(18)O) of short-term (daily) precipitation collected from October 2002 to September 2003 at two stations in a coastal, karstic area in south-western Slovenia was investigated. In addition, monthly composite samples were collected and analysed for comparison with amount-weighted monthly means. The delta(2)H and delta(18)O values obtained show a wide range and reflect seasonal climatic variations. Deuterium excess and local meteoric water lines (LMWLs) were determined and cumulative frequency analysis and coincidence tests were performed. The statistical coincidence test showed that the LMWLs calculated from monthly data for Portoroz and Kozina are coincident, but the LMWLs calculated from daily precipitation events are not. This difference could be explained by the greater variance of the isotopic composition of daily precipitation in comparison to monthly composite samples and also to the influence of evaporation during events below<1 mm at Portoroz during the extremely dry and warm spring-summer season of 2003. Finally, synoptic maps and backward trajectories of a selected precipitation event showed that changes of isotopic composition are related to mixing of air masses originating from the continent and Mediterranean cyclogenesis.     

Influence of the isotopic composition of Li, Rb, and Ag on the absorption of their resonance lines

For the resonance lines of the two-isotope elements Li, Rb, and Ag an investigation is made of the influence of the isotopic composition (b) of an absorbing layer on the magnitude of absorption (A). It is assumed that the contours of the superfine structure (SS) components are of Doppler type and that the source of the line spectrum contains elements of natural isotopic composition. It is shown that A=f(b) for the LiI 670.8 nm line is characterized by a one-to-one dependence on b, and for the RbI 780 nm line it passes through a maximum. For the AgI 383.3 nm line with overlapping SS components the dependence of A on b is practically absent. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 67, No. 2, pp. 251–252, March–April, 2000.     

Nitrogen-15 fractionation in the thermal decomposition of nitrous oxide of natural isotopic composition

The 15N fractionation in the thermal decomposition of nitrous oxide (N2O) of natural isotopic composition has been investigated in quartz reaction vessel in the temperature interval 888-1073 K. The formulas relating the observed experimentally 15N fractionations with the primary 15N kinetic isotope effect, (k14/k15)p for 14N15N16O, and secondary 15N kinetic isotope effect, (k14/k15)s for 15N14N16O, have been derived. The experimentally estimated 15N kinetic isotope effects have been compared with the primary and secondary 15N kinetic isotope effects calculated with the absolute rate theory formulations applied to linear three atom molecules. A good agreement was found for the primary 15N kinetic isotope effect, (k14/k15)p, in the temperature interval 888-1007 K. But at 1073 K the decompositions of N2O, accompanied by NO (nitric oxide) formation proceed with a twice times smaller primary kinetic isotope effect, (k14/k15)p of 1.0251 +/- 0.0009, only, suggesting the nonlinear transition state structures with participation of the fourth external atom at high temperature decompositions of nitrous oxide. The nitrogen isotope effects determined in this study correlate well with nitrogen isotope fractionations observed in the natural biological, earth and atmospheric processes.     

Spectroscopic determination of the nitrogen isotopic composition in the region of subnatural15N concentrations

Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 50, No. 3, pp. 407–412, March, 1989.     

Changes in the surface phase composition of sulfide minerals upon irradiation by high-power nanosecond pulses

The effect of high-power (high-voltage) nanosecond pulses on the phase composition and chemical state of atoms of surface layers of sulfide minerals with different semiconductor properties (galenite, molybdenite, and sphalerite) is investigated by means of XPES. Common patterns and characteristic features of the structural phase transformations of sulfide surfaces under the pulsed energetic effect are the formation and growth of a surface layer by the nonstoichiometric sulfur-enriched sulfide phase and Zn and Mo oxides and hydroxides; the staged character of the transformation of sulfur atoms in the composition of galenite and sphalerite surface layers; and the stability of the chemical state of sulfur in the molybdenite composition and lead atoms in the galenite composition.     

Measuring the isotopic composition of superheavy nuclei of galactic cosmic rays in the NUCLEON-2 experiment

A brief survey of the data on the isotopic composition of superheavy nuclei in galactic cosmic rays is presented. The scientific goals of the planned experiment are outlined, and the design of the NUCLEON-2 scientific equipment is given.     

Diurnal variations in the photosynthesis-respiration activity of a cyanobacterial bloom in a freshwater dam reservoir: an isotopic study

The stable isotopic analyses of molecular oxygen dissolved in water (delta18O(DO)) and dissolved inorganic carbon (delta13C(DIC)), supplemented with basic chemical measurements, have been carried out on a diurnal basis to better understand the dynamics of photosynthesis and respiration in freshwater systems. Our observations have been carried out in a lowland dam reservoir, the Sulejow Lake (central Poland), during the summer cyanobacterial bloom. All data obtained, isotopic, hydrochemical, and biological, show a high mutual consistency. Namely, the lowest delta18O(DO) values, obtained at 10:00 and 14:00 (16.0 and 15.5 per thousand, respectively), correspond to the highest amount of cyanobacterial cells observed (66 and 63 mg dm(-3), respectively), whereas the minimum delta13C(DIC) (-10.6 per thousand) obtained at 22:00 corresponds to the maximum content of organic matter (110 mg dm(-3)). This evidence suggests that isotopic assays of delta18O(DO) and delta13C(DIC) are a reliable tool for the quantitative study of biochemical processes in freshwater systems.     

Aromatic hydrocarbons in the rocks and minerals of hydrothermal deposits (as exemplified by the Darasun gold deposit in the eastern Transbaikal region)

Polycyclic aromatic hydrocarbons found in the rocks and minerals of the Darasun deposit were identified on the basis of their quasi-line spectra. The quantitative determination of the aromatic hydrocarbons made it possible to establish a genetic link between the hydrocarbons and the latter phases of the hydrothermal process. The results obtained agree well with data obtained by the luminescence-bituminological method.     

Sulphur and oxygen isotopic characters of dissolved sulphate in groundwater from the Pleistocene aquifer in the southern Jordan Valley (Jericho area, Palestine)

Sulphate and chloride concentrations in the shallow Pleistocene aquifer systems in the lower Jordan valley area indicate a general trend of increasing salinity eastward and southward. This study was conducted in one of the important sub-basins feeding the Pleo-Pleistocene aquifer in the Jericho area in the southern part of the valley using S and O isotopes of dissolved sulphate. The results show that sulphate has mainly two contributions to the groundwater. One is the surface seepage, which is present as a salty leachate form with the positive delta34Ssulphate values of primary gypsum in Lisan and Samara formations, and the second is the upwelling saline water which was in contact with a deep secondary gypsum, aragonites and salty rocks and rose up under heavy abstraction with depleted 34S in sulphate and relatively high sulphate and chloride content. The latest was clearly shown in the Arab Project wells to the east that is undergoing a continuous heavy abstraction. The isotopic signatures of S and O in these wells to the east show that this depleted 34S and highly concentrated sulphate might also indicate a dissolved sulphate originating from pyrite oxidation that results from the interaction with a pyrite-rich aquifer, which can well up with salty water under heavy abstraction and is oxidised in the upper aerobic shallow aquifer.     

Evolution of isotopic composition of reprocessed uranium during the multiple recycling in light water reactors with natural uranium feed

A complex approach based on the consistent modeling of neutron-physics processes and processes of cascade separation of isotopes is applied for analyzing physical problems of the multiple usage of reprocessed uranium in the fuel cycle of light water reactors. A number of scenarios of multiple recycling of reprocessed uranium in light water reactors are considered. In the process, an excess absorption of neutrons by the ²³⁶U isotope is compensated by re-enrichment in the ²³⁵U isotope. Specific consumptions of natural uranium for re-enrichment of the reprocessed uranium depending on the content of the ²³²U isotope are obtained.     

Changes in the functional chemical composition of the surfaces and microhardness of kimberlite minerals under the action of nanosecond high voltage pulses

Using a set of physicochemical methods (XPS, analytical electron microscopy, the adsorption of acid–base indicators, and measuring microhardness), the effectiveness of nonthermal action produced by nanosecond high voltage pulses for targeted changes in the phase (functional chemical) composition and technological properties of rock-forming minerals of kimberlites and diamonds is shown. According to data obtained via XPS and SEM-EDX analyses, pulse energy actions damage the surface microstructure of dielectric minerals with the subsequent formation of traces of surface breakdowns and microcracks, softening rockforming minerals, and reducing their microhardness by 40–66% overall. The following changes in the functional chemical composition of a geomaterial surface are established through the adsorption of acid–base indicators: mutual transformations of the Brønsted base, Lewis base, and Brønsted acid sites on a calcite surface under the action of an electromagnetic pulse and the hydroxylation and/or formation of carbonyl groups on a diamond surface, doubling the diamond electrokinetic potential in the negative range.     

Application of diffraction methods to the study of volume variations in the composition of a langatate single crystal

A langatate single crystal with the initial composition La₃Ga_5.5Ta_0.5O₁₄, which is grown by means of Czochralski pulling along the 〈0001〉 direction in a weakly oxidizing medium, is investigated via X-ray and neutron diffraction techniques. The crystal is inhomogeneous in color and composition. The middle part of the single crystal is revealed to have a more homogeneous composition than its upper part. It is demonstrated that the color change depends on the amount of oxygen vacancies in different parts of the single-crystal boule.     

Effect of isotopic composition and microstructure on the crystalline and magnetic phase states in R0.5Sr0.5MnO3

The results of structural neutron experiments on determining crystal and magnetic phase states of perovskite-like manganites R_0.5Sr_0.5MnO₃ (R = ¹⁵²Sm, Nd_0.772Tb_0.228, and Nd_0.544Tb_0.456) are reported. Experiments are carried out for revealing microscopic factors responsible for the giant oxygen isotope effect that was discovered recently in Sm_1?x Sr _x MnO₃ for x ≈ 0.5. It is shown that separation into two crystal phases P ₁ and P ₂ with the same spatial symmetry but different types of Jahn-Teller distortions in MnO₆ octahedra and magnetic ordering of Mn atoms takes place in all studied compounds at low temperatures. Structural analysis has been carried out successfully owing to exceptionally large differences in the unit cell parameters of the coexisting phases. The P ₁ phase is ferromagnetic and MnO₆ octahedra are distorted only slightly. The P ₂ phase is antiferromagnetic (A-type ordering) and MnO₆ octahedra are strongly compressed in the apical direction. The relative volumes occupied by the P ₁ and P ₂ phases depend on the mean radius of the A cation, and the replacement of ¹⁶O by ¹⁸O results in their redistribution in favor of the P ₂ phase. The results unambiguously point to the percolation nature of the metal-insulator transition in a Sm-containing compound upon isotopic substitution of oxygen due to a sharp decrease (from 65 to 13%) in the fraction of ferromagnetic phase P ₁. In all investigated compounds, the ordered magnetic moment of manganese Mn in the P ₁ and P ₂ phases varies from 1.7μ_B to 3.5μ_B. The data on the evolution of the miscrostructure parameters during a phase transition to the stratified state indicate that the initial spread in the A cation radii, as well as the internal microstrains, produce a critical effect on the formation of mesoscopic phase separation.