近垒及垒下能区重离子熔合-裂变反应机制的研究

本工作用固体云母核径迹探测器测量了质心能量为73.7至93.4MeV的~(16)O + ~(238)U和能量为57.9至76.0MeV的~(12)C + ~(237)Np系统熔合裂变碎片角分布和截面；首次用双栅位置灵敏雪崩计数器[DGAC]测量了质心能量为46.5至56.2 MeV的~(11)B + ~(238)U和能量为58.9至76.0 MeV的~(12)C + ~(237)Np及84.0MeV的~(16)O + ~(238)U系统熔合裂变碎片角关联和截面。研究结果表明：使用二种测量方法得到的熔合裂变截面和裂变碎片角分布是一致的，对于三个反应系统熔合裂变截面用考虑靶核形变的耦合道理论能得到合理的描述；而从计算熔合截面中提取穿透系数，从有限力程转动液滴模型中提取有效转动惯量，用鞍点过渡态理论计算裂变碎片角分布，发现裂变碎片角分布各向异性异常；随入射能量减少，各向异性并不是单调地变化，而是呈现异常的“鼓包”；裂变碎片各向异性还有明显的入射道效应，在近垒和垒上能区~(12)C + ~(237)Np和~(11)B + ~(238)U系统裂变碎片角分布可以用鞍点过渡态理论描述，没有发现异常；而对于~(16)O + ~(238)U系统裂变碎片角分布都有大于理论的异常，而且在垒上低能端异性度随能量的变化走向不同于以前测量的结果。虽然入射道效应证明了前平衡裂变的理论预言，但对于垒下能区，碎片异性度的异常依然存在，表明仅用前平衡裂变理论解释裂变碎片角分布的异常是不够的。为了澄清转移裂变对角分布异常的贡献，采用了角关联技术成功地区分出复合核裂变和转移裂变，实现了对纯复合核裂变碎片角分布各向异性的研究。在被研究的能区内，转移裂变占总裂变截面10%以下，而且它的各向异性度比复合核裂变的要小，扣除转移裂变的贡献使裂变碎片异性度提高5%，因此角分布异常不可能起源于转移裂变的贡献

中能重离子反应中靶碎片的质量分布研究

本文利用核化学方法研究了中能重离子反应机制。在135MeV/u~(12)C + Fe反应中鉴别了39个放射性核素，并得到了这些靶余核的生成截面，通过电荷分布假设导出了该反应中靶余核的质量分布。结果表明，中能重离子与非裂变靶核相互作用中靶余核质量分布的形状相似，随着入射能的增加，质量分布曲线变得更加平缓。同时，在低质量区（A < 30）反应产物的产额明显增加，且产物有偏向丰中子一侧的趋势。利用熔合碎裂统计模型和级联两体统计模型对实验结果进行了拟合，两种理论模型都能较好地符合实验数据的总体趋势，但考虑了多重碎裂衰变模式的熔合碎裂统计模型的计算结果再现了A < 30质量区产额的回升现象，而级联两体模型更好地符合了蒸发余核的质量分布，预示着在很高入射能的情况下，多重碎裂成为靶余核形成的主要反应机制之一。在20MeV/u~(40)Ar引起~(238)U的裂变反应中测到了101个核素的生成截面，通过高斯电荷分布曲线拟合得到了各同量民位素的独立产额以及各质量链的质量产额。从电荷分布曲线中可以看出，裂变碎片来源于两种不同的反应机制，即丰中子产物来自高激发核的裂变过程，而缺中子产物来自低能裂变过程。质量分布曲线在裂变质量区（80 < A < 140）有一很宽的对称裂变峰而在近靶区的重靶余核也能以很高的截面通过周边碰撞产生

Fragment mass distributions in the fission of heavy nuclei by intermediate- and high-energy probes

Recent experiments have shown that the multimode approach for describing the fission process is compatible with the observed results. Asystematic analysis of the parameters obtained by fitting the fission-fragment mass distribution to the spontaneous and low-energy data has shown that the values for those parameters present a smooth dependence upon the nuclear mass number. In this work, a new methodology is introduced for studying fragment mass distributions through the multimode approach. It is shown that for fission induced by energetic probes (E > 30 MeV) the mass distribution of the fissioning nuclei produced during the intranuclear cascade and evaporation processes must be considered in order to have a realistic description of the fission process. The method is applied to study (208)Pb, (238)U, (239)Np and (241)Am fission induced by protons or photons.

Sub-barrier fusion of two-neutron halo nuclei

The tunneling of composite systems, where breakup may occur during the barrier penetration process, is considered in connection with the fusion of halo-like radioactive, neutron- and proton-rich nuclei, on heavy targets. The large amount of recent and new data clearly indicates that breakup hinders the fusion at energies near and below the Coulomb barrier. However, clear evidence for enhancement due to halo properties seems to over ride the breakup hindrance at lower energies, owing, to a large extent, to the extended matter density distribution. In particular we report here that at sub-barrier energies the fusion cross section of the Borromean two-neutron halo nucleus (6)He with the actinide nucleus (238)U is significantly enhanced as compared to the fusion of a similar projectile with no halo. This conclusion differs from that of the original work, where it was claimed that no such enhancement ensues. This sub-barrier fusion enhancement is also observed in the (6)He + (209)Bi system. (C) 2010 Elsevier B.V. All rights reserved.

Universal trend for heavy-ion total reaction cross-sections at energies above the Coulomb barrier

Heavy-ion total reaction cross-section measurements for more than 1100 reaction cases covering 61 target nuclei in the range (6)Li-(238)U and 158 projectile nuclei from (2)H to (84)Kr (mostly exotic ones) have been analyzed in a systematic way by using an empirical, three-parameter formula that is applicable to the cases of projectile kinetic energies above the Coulomb barrier. The analysis has shown that the average total nuclear binding energy per nucleon of the interacting nuclei and their radii are the chief quantities that describe the cross-section patterns. A great amount of cross-section data (87%) has been quite satisfactorily reproduced by the proposed formula; therefore, the total reaction cross-section predictions for new, not yet experimentally investigated reaction cases can be obtained within 25% (or much less) uncertainty.

Chemical and radiological characterization of clay minerals used in pharmaceutics and cosmetics

Since the early days, clays have been used for therapeutic purposes. Nowadays, they are used as active ingredients or as excipient in formulations for a variety of purposes. Despite their wide use, little information is available in literature on their content of trace elements and radionuclides. The purpose of this study was to determine the elements (As, Ba, Br, Cs, Co, Cr, Eu, Fe, Hf, Hg, La, Lu, Rb, Sb, Sc, Sm, Ta, Tb, Yb, Zn, and Zr) and the radionuclides ((238)U, (232)Th, (226)Ra, (228)Ra, (210)Pb and (40)K) in Brazilian clays as well as the health and radiological implications of the use of these clays in pharmaceutical formulations. (C) 2011 Elsevier B.V. All rights reserved.

Group analysis method for fission track thermochronology

A methodology to obtain ages and thermal histories of sets of apatite samples from localities with geologically compatible characteristics is described. A methodology exploring the fact that samples with similar geological characteristics should present the same thermal history is proposed. This approach can contribute for the obtainment of more conclusive results by analysing fewer samples than it is necessary when the samples are individually analysed. In order to determine the ages, we use the absolute neutron dosimetry through thin films of natural uranium along with lambda(f) = 8.46 x 10(-17) a(-1). As an example of application of the proposed methodology, we analyse samples collected in a Brazilian region, Sao Francisco Craton, which experienced low tectonic activity. (C) 2008 Elsevier Ltd. All rights reserved.

Hydro(radio)chemical relationships in the giant Guarani aquifer, Brazil

This investigation was carried out within the Parana sedimentary basin and involved the sampling of 78 pumped tubular wells for evaluating the hydrochemistry and radioactivity due to the nuclides (238)U, (234)U, (222)Ra, (226)Ra, and (228)Ra in the Brazilian part of Guarani aquifer. Several significant correlations were found involving the geostatic pressure, for instance, specific flow rate, CO(3)(2-), SO(4)(2-) temperature, dissolved O(2), free CO(2), pH, redox potential Eh, conductivity, Na, HCO(3)-, CO(3)(2-) , SI(calcite), Cl(-), F(-), SO(4)(2-), and B. Carbonates precipitation was evidenced by inverse correlation between CO(3)(2-) and Ca, Mg, Sr, and Ba, whereas Na exhibited an opposite trend, dissolving rather than precipitating with increasing CO(3)(2-) concentration. An inverse correlation between 3 and K was found, possibly related to the increasing tendency of K to recombine with the thickness of the clayey layers. HCO(3)-played an important role on Na, Ca, Mg, and Sr dissolution. The dissolved U content and (234)U/(238)U activity ratio data were plotted on a two-dimensional diagram that was successfully utilized on identifying an unreported zone of U accumulation, though not necessarily of economic size and grade. The variability in chemical and radionuclides data indicated an important influence of the underlying Paleozoic sediments in the composition of waters from Guarani aquifer. The available data allowed estimate the groundwater residence time by two U-isotopes disequilibrium methods. Values of 45-61 ka were initially calculated, depending on the adopted porosity (15-20%), but a longer residence time (- 640 ka) was also estimated, which is more compatible with the hydraulic conductivity data in Guarani aquifer and groundwater flow velocity occurring at Milk River aquifer, Alberta, Canada. Such time range agrees with previously reported (14)C ages exceeding 30 ka BP at the more central parts of the Parana sedimentary basin. (c) 2005 Elsevier B.V. All rights reserved.

The natural radioactivity in Guarani aquifer groundwater, Brazil

Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)

Natural radionuclides in major aquifer systems of the Parana sedimentary basin, Brazil

Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)

Radionuclide concentrations in raw and purified phosphoric acids from Brazil and their processing wastes: implications for radiation exposures

Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)

Potentialities and practical limitations of absolute neutron dosimetry using thin films of uranium and thorium applied to the fission track dating

Neutron dosimetry using natural uranium and thorium thin films makes possible that mineral dating by the fission-track method can be accomplished, even when poor thermalized neutron facilities are employed. In this case, the contributions of the fissions of (235)U, (238)U and (232)Th induced by thermal, epithermal and fast neutrons to the population of tracks produced during irradiation are quantified through the combined use of natural uranium and thorium films.If the Th/U ratio of the sample is known, only one irradiation (where the sample and the films of uranium and thorium are present) is necessary to perform the dating. However, if that ratio is unknown, it can be determined through another irradiation where the mineral to be dated and both films are placed inside a cadmium box.Problems related with film manufacturing and calibration are discussed. Special attention is given to the utilization of thin films having very low uranium content. The problems faced suggest that it may be better to substitute these films by uranium doped standard glasses calibrated with thicker uranium films (thickness greater than 1.5 x 10(13) mu m).

Radionuclides, heavy metals and fluorine incidence at Tapira phosphate rocks, Brazil, and their industrial (by) products

Inorganic phosphate fertilizers may contain radionuclides, heavy metals and fluorine. This paper presents the possible environmental hazards from Tapira phosphate rocks and their (by) products (Brazil) utilized as phosphate fertilizers. The activity concentration of U-238, U-234, Ra-226 and K-40 in Tapira phosphate rocks is within the world range for these rock types. The Th-232 activity concentration is higher than the mean reported in phosphate rocks. A value of 2184 nGy h(-1) was obtained for the exposure dose rate in Tapira phosphate deposit area, which is indicative of a high background radiation area. The flotation-separation process causes the incorporation of no more than 9%, 11 % and 24% of radionuclides, heavy metals and fluorine, respectively, into the phosphate concentrate. The radionuclides and heavy metals existing in phosphate fertilizers applied in Brazilian crops according to the recommended rates, do not raise their concentration in soils to harmful levels. (C) 2005 Elsevier Ltd. All rights reserved.

Seleção de linhagens de basidiomicetos resistentes aos herbicidas atrazina e diurom -produção de enzimas ligninolíticas e degradação dos compostos

Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)

Diffusion-driven transport in clayrock formations

Clay mineral-rich sedimentary formations are currently under investigation to evaluate their potential use as host formations for installation of deep underground disposal facilities for radioactive waste (e.g. Boom Clay (BE), Opalinus Clay (CH), Callovo-Oxfordian argillite (FR)). The ultimate safety of the corresponding repository concepts depends largely on the capacity of the host formation to limit the flux towards the biosphere of radionuclides (RN) contained in the waste to acceptably low levels. Data for diffusion-driven transfer in these formations shows extreme differences in the measured or modelled behaviour for various radionuclides, e. g. between halogen RN (Cl-36, I-129) and actinides (U-238,U-235, Np-237, Th-232, etc.), which result from major differences between RN of the effects on transport of two phenomena: diffusion and sorption. This paper describes recent research aimed at improving understanding of these two phenomena, focusing on the results of studies carried out during the EC Funmig IP on clayrocks from the above three formations and from the Boda formation (HU). Project results regarding phenomena governing water, cation and anion distribution and mobility in the pore volumes influenced by the negatively-charged surfaces of clay minerals show a convergence of the modelling results for behaviour at the molecular scale and descriptions based on electrical double layer models. Transport models exist which couple ion distribution relative to the clay-solution interface and differentiated diffusive characteristics. These codes are able to reproduce the main trends in behaviour observed experimentally, e.g. D-e(anion) < D-e(HTO) < D-e(cation) and D-e(anion) variations as a function of ionic strength and material density. These trends are also well-explained by models of transport through ideal porous matrices made up of a charged surface material. Experimental validation of these models is good as regards monovalent alkaline cations, in progress for divalent electrostatically-interacting cations (e.g. Sr2+) and still relatively poor for 'strongly sorbing', high K-d cations. Funmig results have clarified understanding of how clayrock mineral composition, and the corresponding organisation of mineral grain assemblages and their associated porosity, can affect mobile solute (anions, HTO) diffusion at different scales (mm to geological formation). In particular, advances made in the capacity to map clayrock mineral grain-porosity organisation at high resolution provide additional elements for understanding diffusion anisotropy and for relating diffusion characteristics measured at different scales. On the other hand, the results of studies focusing on evaluating the potential effects of heterogeneity on mobile species diffusion at the formation scale tend to show that there is a minimal effect when compared to a homogeneous property model. Finally, the results of a natural tracer-based study carried out on the Opalinus Clay formation increase confidence in the use of diffusion parameters measured on laboratory scale samples for predicting diffusion over geological time-space scales. Much effort was placed on improving understanding of coupled sorption-diffusion phenomena for sorbing cations in clayrocks. Results regarding sorption equilibrium in dispersed and compacted materials for weakly to moderately sorbing cations (Sr2+, Cs+, Co2+) tend to show that the same sorption model probably holds in both systems. It was not possible to demonstrate this for highly sorbing elements such as Eu(III) because of the extremely long times needed to reach equilibrium conditions, but there does not seem to be any clear reason why such elements should not have similar behaviour. Diffusion experiments carried out with Sr2+, Cs+ and Eu(III) on all of the clayrocks gave mixed results and tend to show that coupled diffusion-sorption migration is much more complex than expected, leading generally to greater mobility than that predicted by coupling a batch-determined K-d and Ficks law based on the diffusion behaviour of HTO. If the K-d measured on equivalent dispersed systems holds as was shown to be the case for Sr, Cs (and probably Co) for Opalinus Clay, these results indicate that these cations have a D-e value higher than HTO (up to a factor of 10 for Cs+). Results are as yet very limited for very moderate to strongly sorbing species (e.g. Co(II), Eu(III), Cu(II)) because of their very slow transfer characteristics. (C) 2011 Elsevier Ltd. All rights reserved.