315 resultados para 238U


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Terrestrial radioactivity for most individual is the major contributor to the total dose and is mostly provided by 238U, 232Th and 40K radionuclides. In particular indoor radioactivity is principally due to 222Rn, a radioactive noble gas descendent of 238U, second cause of lung cancer after cigarettes smoking. Vulsini Volcanic District is a well known quaternary volcanic area located between the northern Latium and southern Tuscany (Central Italy). It is characterized by an high natural radiation background resulting from the high concentrations of 238U, 232Th and 40K in the volcanic products. In this context, subduction-related metasomatic enrichment of incompatible elements in the mantle source coupled with magma differentiation within the upper crust has given rise to U, Th and K enriched melts. Almost every ancient village and town located in this part of Italy has been built with volcanic rocks pertaining to the Vulsini Volcanic District. The radiological risk of living in this area has been estimated considering separately: a. the risk associated with buildings made of volcanic products and built on volcanic rock substrates b. the risk associated to soil characteristics. The former has been evaluated both using direct 222Rn indoor measurements and simulations of “standard rooms” built with the tuffs and lavas from the Vulsini Volcanic District investigated in this work. The latter has been carried out by using in situ measurements of 222Rn activity in the soil gases. A radon risk map for the Bolsena village has been developed using soil radon measurements integrating geological information. Data of airborne radioactivity in ambient aerosol at two elevated stations in Emilia Romagna (North Italy) under the influence of Fukushima plume have been collected, effective doses have been calculated and an extensive comparison between doses associated with artificial and natural sources in different area have been described and discussed.

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Le attuali sezioni d’urto di reazioni indotte da neutroni non sono sufficientemente accurate per essere utilizzate in progetti di ricerca di frontiera. Per soddisfare la richiesta di nuovi dati nucleari è stata recentemente costruita al CERN di Ginevra la facility n_TOF (neutron Time Of Flight). Le caratteristiche che contraddistinguono questa facility sono l’elevato flusso istantaneo di neutroni, l’ampio spettro energetico e l’eccellente risoluzione energetica. In questa tesi viene analizzata la sezione d’urto di cattura neutronica su 238U, fondamentale per la realizzazione dei reattori nucleari di nuova generazione che prevedono la sostituzione del combustibile 235U con 238U, molto più abbondante in natura e che permette di ridurre drasticamente l’accumulo di scorie nucleari. Nonostante le numerose misure già effettuate su questo elemento, ancora non si è raggiunta la precisione necessaria per le tecnologie nucleari emergenti quali i reattori di quarta generazione e gli ADS (Accelerator Drive System). Inoltre la parametrizzazione della sezione d’urto in termini di matrice R, non è così accurata quanto richiesto. In questo lavoro si è dapprima studiata l’assegnazione dello spin delle risonanze riportata in letteratura, elemento fondamentale per la successiva analisi delle risonanze e la parametrizzazione della sezione d’urto della reazione 238U(n, ). Parallelamente a questa attività si è studiata la funzione di risposta dello spettrometro n_TOF, che descrive la risoluzione energetica dei neutroni incidenti e va quindi a modificare la forma delle risonanze. I risultati ottenuti sono quindi stati confrontati con quelli in letteratura per poter essere validati e per poter verificare eventuali migliorie.

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In dieser Arbeit wird die Erweiterung und Optimierung eines Diodenlasersystems zur hochauflösenden Resonanzionisationsmassenspektrometrie beschrieben. Ein doppelinterferometrisches Frequenzkontrollsystem, welches Absolutstabilisierung auf ca. 1 MHz sowie sekundenschnelle Frequenzverstimmungen um mehrere GHz für bis zu drei Laser parallel ermöglicht, wurde optimiert. Dieses Lasersystem dient zwei wesentlichen Anwendungen. Ein Aspekt waren umfangreiche spektroskopische Untersuchungen an Uranisotopen mit dem Ziel der präzisen und eindeutigen Bestimmung von Energielagen, Gesamtdrehimpulsen, Hyperfeinkonstanten und Isotopieverschiebungen sowie die Entwicklung eines effizienten, mit kommerziellen Diodenlasern betreibbaren Anregungsschemas. Mit diesen Erkenntnissen wurde die Leistungsfähigkeit des Lasermassenspektrometers für die Ultraspurenanalyse des Isotops 236U, welches als Neutronendosimeter und Tracer für radioaktive anthropogene Kontaminationen in der Umwelt verwendet wird, optimiert und charakterisiert. Anhand von synthetischen Proben wurde eine Isotopenselektivität von 236U/238U=4,5(1,5)∙10-9 demonstriert.

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Kalorimetrische Tieftemperatur-Detektoren (Calorimetric Low Temperature Detectors, CLTDs) wurden erstmals in Messungen zur Bestimmung des spezifischen Energieverlustes (dE/dx) niederenergetischer Schwerionen beim Durchgang durch Materie eingesetzt. Die Messungen wurden im Energiebereich unterhalb des Bragg-Peaks, mit 0.1 - 1.4 MeV/u 238U-Ionen in Kohlenstoff und Gold sowie mit 0.05 - 1.0 MeV/u 131Xe-Ionen in Kohlenstoff, Nickel und Gold, durchgeführt. Die Kombination der CLTDs mit einem Flugzeitdetektor ermöglichte dabei, kontinuierliche dE/dx-Kurven über größere Energiebereiche hinweg simultan zu bestimmen. Im Vergleich zu herkömmlichen Meßsystemen, die Ionisationsdetektoren zur Energiemessung verwenden, erlaubten die höhere Energieauflösung und -linearität der CLTDs eine Verringerung der Kalibrierungsfehler sowie eine Erweiterung des zugänglichen Energiebereiches der dE/dx-Messungen in Richtung niedriger Energien. Die gewonnen Daten können zur Anpassung theoretischer und semi-empirischer Modelle und somit zu einer Erhöhung der Präzision bei der Vorhersage spezifischer Energieverluste schwerer Ionen beitragen. Neben der experimentellen Bestimmung neuer Daten wurden das alternative Detektionsprinzip der CLTDs, die Vorteile dieser Detektoren bezüglich Energieauflösung und -linearität sowie der modulare Aufbau des CLTD-Arrays aus mehreren Einzeldetektoren genutzt, um diese Art von Messung auf potentielle systematische Unsicherheiten zu untersuchen. Unter anderem wurden hierbei unerwartete Channeling-Effekte beim Durchgang der Ionen durch dünne polykristalline Absorberfolien beobachtet. Die koinzidenten Energie- und Flugzeitmessungen (E-ToF) wurden weiterhin genutzt, um das Auflösungsvermögen des Detektor-Systems bei der direkten in-flight Massenbestimmung langsamer und sehr schwerer Ionen zu bestimmen. Durch die exzellente Energieauflösung der CLTDs konnten hierbei Massenauflösungen von Delta-m(FWHM) = 1.3 - 2.5 u für 0.1 - 0.6 MeV/u 238U-Ionen erreicht werden. In einer E-ToF-Messung mit Ionisationsdetektoren sind solche Werte in diesem Energie- und Massenbereich aufgrund der Limitierung der Energieauflösung durch statistische Schwankungen von Verlustprozessen beim Teilchennachweis nicht erreichbar.

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The occurrence of elevated uranium (U) in sandstone aquifers was investigated in the Upper Peninsula of Michigan, focusing on aquifers of the Jacobsville Sandstone. The hydrogeochemical controls on groundwater U concentrations were characterized using a combination of water sampling and spectral gamma-ray logging of sandstone cliffs and residential water wells. 235U/238U isotope ratios were consistent with naturally occurring U. Approximately 25% of the 270 wells tested had U concentrations above the U.S. Environmental Protection Agency Maximum Contaminant Level (MCL) of 30 μg/L, with elevated U generally occurring in localized clusters. Water wells were logged to determine whether groundwater U anomalies could be explained by the heterogeneous distribution of U in the sandstone. Not all wells with relative U enrichment in the sandstone produced water with U above the MCL, indicating that the effect of U enrichment in the sandstone may be modified by other hydrogeochemical factors. Well water had high redox, indicating U is in its highly soluble (VI) valence. Equilibrium modeling indicated that aqueous U is complexed with carbonates. In general, wells with elevated U concentrations had low 235U/238U activity ratios. However, in some areas U concentrations and 235U/238U activity ratios were simultaneously high, possibly indicating differences in rock-water interactions. Limited groundwater age dating suggested that residence time may also help explain variations in well water U concentrations. Low levels of U enrichment (4 to 30 ppm) in the Jacobsville sandstone may make wells in its oxidized aquifers at risk for U concentrations above the MCL. On average, U concentrations were highest in heavy mineral and clay layers and rip up conglomerates. Uranium concentrations above 4 ppm also occurred in siltstones, sandstones and conglomerates. Uranium enrichment was likely controlled by deposition processes, sorption to clays, and groundwater flow, which was controlled by permeability variations in the sandstone. Low levels of U enrichment were found at deltaic, lacustrine and alluvial fan deposits and were not isolated to specific depositional environments.

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Fission fragment mass distributions were measured in heavy-ion induced fission of 238U. The mass distributions changed drastically with incident energy. The results are explained by a change of the ratio between fusion and quasifission with nuclear orientation. A calculation based on a fluctuation dissipation model reproduced the mass distributions and their incident energy dependence. Fusion probability was determined in the analysis. Evaporation residue cross sections were calculated with a statistical model for the reactions of 30Si+238U and 34S+238U using the obtained fusion probability in the entrance channel. The results agree with the measured cross sections of 263,264Sg and 267,268Hs, produced by 30Si+238U and 34S+238U, respectively. It is also suggested that sub-barrier energies can be used for heavy element synthesis.

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The Central gold belt of peninsular Malaysia comprises a number of gold deposits located in the east of the N-S striking Bentong-Raub Suture Zone. The Tersang gold deposit is one of the gold deposits in the gold belt and hosted in sandstone, rhyolite and breccia units. The deposit has an inferred resource of 528,000 ounces of gold. The geochronology of the Tersang deposit has been newly constrained by LA ICP-MS U-Pb zircon dating. The maximum depositional age of the host sedimentary rocks ranges from Early Carboniferous to Early Permian (261.5 ± 4.9 Ma to 333.5 ± 2.5 Ma) for the host sandstone and Late Triassic for the rhyolite intrusion (218.8 ± 1.7 Ma). Textural characteristics of pyrite have revealed five types including (1) Euhedral to subhedral pyrite with internal fracturing and porous cores located in the sandstone layers (pyrite 1); (2) Anhedral pyrite overgrowths on pyrite 1 and disseminated in stage 1 vein (pyrite 2); (3) Fracture-filled or vein pyrite located in stages 1 and 2 vein (pyrite 3); (4) Euhedral pyrite with internal fractures also located in stage 2 vein (pyrite 4); and (5) Subhedral clean pyrite located in the rhyolite intrusion (pyrite 5). Based on pyrite mapping and spot analyses, two main stages of gold enrichment are documented from the Tersang gold deposit. Gold in sandstone-hosted pyrite 1 (mean 4.3 ppm) shows best correlation with Bi and Pb (as evidenced on pyrite maps). In addition, gold in pyrite 3 (mean 8 ppm) located in stage 2 vein shows a good correlation with As, Ag, Sb, Cu, Tl, and Pb. In terms of gold exploration, we suggest that elements such as As, Ag, Sb, Cu, Tl, Bi, and Pb associated with Au may serve as vectoring tools in gold exploration. Our new geological, structural, geochemical and isotopic data together with mineral paragenesis, pyrite chemistry and ore fluid characteristics indicate that the Tersang gold deposit is comparable to a sediment-hosted gold deposit. Our new genetic model suggests deposition of the Permo-Carboniferous sediments followed by intrusion of rhyolitic magma in the Late Triassic. At a later stage, gold mineralisation overprinted the rhyolite intrusion and the sandstone.

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Tropical south-western Pacific temperatures are of vital importance to the Great Barrier Reef (GBR), but the role of sea surface temperatures (SSTs) in the growth of the GBR since the Last Glacial Maximum remains largely unknown. Here we present records of Sr/Ca and d18O for Last Glacial Maximum and deglacial corals that show a considerably steeper meridional SST gradient than the present day in the central GBR. We find a 1-2 °C larger temperature decrease between 17° and 20°S about 20,000 to 13,000 years ago. The result is best explained by the northward expansion of cooler subtropical waters due to a weakening of the South Pacific gyre and East Australian Current. Our findings indicate that the GBR experienced substantial meridional temperature change during the last deglaciation, and serve to explain anomalous deglacial drying of northeastern Australia. Overall, the GBR developed through significant SST change and may be more resilient than previously thought.

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We present uranium-thoriumchronology for a 102 mcore through a Pleistocene reef at Tahiti (French Polynesia) sampled during IODP Expedition 310 "Tahiti Sea Level". We employ total and partial dissolution procedures on the older coral samples to investigate the diagenetic overprint of the uranium-thoriumsystem. Although alteration of the U-Th system cannot be robustly corrected, diagenetic trends in the U-Th data, combined with sea level and subsidence constraints for the growth of the corals enables the age of critical samples to be constrained to marine isotope stage 9. We use the ages of the corals, together with d18O based sea-level histories, to provide maximum constraints on possible paleo water-depths. These depth constraints are then compared to independent depth estimates based on algal and foraminiferal assemblages, microbioerosion patterns, and sedimentary facies, confirming the accuracy of these paleo water-depth estimates. We also use the fact that corals could not have grown above sea level to place amaximumconstraint on the subsidence rate of Tahiti to be 0.39 m ka**-1,with the most likely rate being close to the existing minimum estimate of 0.25m ka**-1.

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The ESR dating method was applied to marine shells taken from a sediment core from Dagebüll, Schleswig-Holstein. Four samples from two different depths of the core (17.5 m and 25-26 m), separated by a 2.76 meter thick clay layer (Turritella Clay), yielded identical ages within the limits of error. They indicated an assignment to the oxygen isotope stage 5, thus confirming the stratigraphic age. In addition, the ESR-ages confirm the interpretation of Lomitschka et al. (1997, doi:10.2312/meyniana.1997.49.85), that the Th/U-ages of shells below the clay layer are reliable, whereas shells located above the clay layer, which were strongly influenced by percolating groundwaters of an open system, yielded falsified Th/U-ages.

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A limiting factor in the accuracy and precision of U/Pb zircon dates is accurate correction for initial disequilibrium in the 238U and 235U decay chains. The longest-lived-and therefore most abundant-intermediate daughter product in the 235U isotopic decay chain is 231Pa (T1/2 = 32.71 ka), and the partitioning behavior of Pa in zircon is not well constrained. Here we report high-precision thermal ionization mass spectrometry (TIMS) U-Pb zircon data from two samples from Ocean Drilling Program (ODP) Hole 735B, which show evidence for incorporation of excess 231Pa during zircon crystallization. The most precise analyses from the two samples have consistent Th-corrected 206Pb/238U dates with weighted means of 11.9325 ± 0.0039 Ma (n = 9) and 11.920 ± 0.011 Ma (n = 4), but distinctly older 207Pb/235U dates that vary from 12.330 ± 0.048 Ma to 12.140 ± 0.044 Ma and 12.03 ± 0.24 to 12.40 ± 0.27 Ma, respectively. If the excess 207Pb is due to variable initial excess 231Pa, calculated initial (231Pa)/(235U) activity ratios for the two samples range from 5.6 ± 1.0 to 9.6 ± 1.1 and 3.5 ± 5.2 to 11.4 ± 5.8. The data from the more precisely dated sample yields estimated DPazircon/DUzircon from 2.2-3.8 and 5.6-9.6, assuming (231Pa)/(235U) of the melt equal to the global average of recently erupted mid-ocean ridge basaltic glasses or secular equilibrium, respectively. High precision ID-TIMS analyses from nine additional samples from Hole 735B and nearby Hole 1105A suggest similar partitioning. The lower range of DPazircon/DUzircon is consistent with ion microprobe measurements of 231Pa in zircons from Holocene and Pleistocene rhyolitic eruptions (Schmitt (2007; doi:10.2138/am.2007.2449) and Schmitt (2011; doi:10.1146/annurev-earth-040610-133330)). The data suggest that 231Pa is preferentially incorporated during zircon crystallization over a range of magmatic compositions, and excess initial 231Pa may be more common in zircons than acknowledged. The degree of initial disequilibrium in the 235U decay chain suggested by the data from this study, and other recent high precision datasets, leads to resolvable discordance in high precision dates of Cenozoic to Mesozoic zircons. Minor discordance in zircons of this age may therefore reflect initial excess 231Pa and does not require either inheritance or Pb loss.

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A down-core 231Pa/230Th record has been measured from the southwestern Indian Ocean to reconstruct the history of deep water flow into this basin over the last glacial-interglacial cycle. The (231Paxs/230Thxs)0 ratio throughout the record is nearly constant at approximately 0.055, significantly lower than the production ratio of 0.093, indicating that the proxy is sensitive to changes in circulation and/or sediment flux at this site. The consistent value suggests that there has been no change in the inflow of Antarctic Bottom Water to the Indian Ocean during the last 140 ka, in contrast to the changes in deep circulation thought to occur in other ocean basins. The stability of the (231Paxs/230Thxs)0 value in the record contrasts with an existing sortable silt (SS) record from the same core. The observed equation image variability is attributed to a local geostrophic effect amplifying small changes in circulation. A record of authigenic U from the same core suggests that there was reduced oxygen in bottom waters at the core locality during glacial periods. The consistency of the (231Paxs/230Thxs)0 record implies that this could not have arisen by local changes in productivity, thus suggesting a far-field control: either globally reduced bottom water oxygenation or increased productivity south of the Opal Belt during glacials.

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Seasonal patterns in the partitioning of phytoplankton carbon during receding sea ice conditions in the eastern Bering Sea water column are presented using rates of 14C net primary productivity (NPP), phototrophic plankton carbon content, and POC export fluxes from shelf and slope waters in the spring (March 30-May 6) and summer (July 3-30) of 2008. At ice-covered and marginal ice zone (MIZ) stations on the inner and middle shelf in spring, NPP averaged 76 ± 93 mmol C/m**2/d, and in ice-free waters on the outer shelf NPP averaged 102 ± 137 mmol C/m**2/d. In summer, rates of NPP were more uniform across the entire shelf and averaged 43 ± 23 mmol C/m**2/d over the entire shelf. A concomitant shift was observed in the phototrophic pico-, nano-, and microplankton community in the chlorophyll maximum, from a diatom dominated system (80 ± 12% autotrophic C) in ice covered and MIZ waters in spring, to a microflagellate dominated system (71 ± 31% autotrophic C) in summer. Sediment trap POC fluxes near the 1% PAR depth in ice-free slope waters increased by 70% from spring to summer, from 10 ± 7 mmol C/m**2/d to 17 ± 5 mmol C/m**2/d, respectively. Over the shelf, under-ice trap fluxes at 20 m were higher, averaging 43 ± 17 mmol C/m**2/d POC export over the shelf and slope estimated from 234Th deficits averaged 11 ± 5 mmol C/m**2/d in spring and 10 ± 2 mmol C/m**2/d in summer. Average e-ratios calculated on a station-by-station basis decreased by ~ 30% from spring to summer, from 0.46 ± 0.48 in ice-covered and MIZ waters, to 0.33 ± 0.26 in summer, though the high uncertainty prevents a statistical differentiation of these data.

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The subarctic North Pacific Ocean holds a large CO2 reservoir that is currently isolated from the atmosphere by a low-salinity layer. It has recently been hypothesized that the reorganization of these high-CO2 waters may have played a crucial role in the degassing of carbon dioxide to the atmosphere during the last deglaciation. This reorganization would leave some imprint on paleo-productivity records. Here we present 230Th-normalized biogenic fluxes from an intermediate depth sediment core in the Northwest Pacific (RC10-196, 54.7°N, 177.1°E, 1007 m) and place them within the context of a synthesis of previously-published biogenic flux data from 49 deep-sea cores north of 20°N, ranging from 420 to 3968 m water depth. The 230Th-normalized opal, carbonate, and organic carbon fluxes from RC10-196 peak approximately 13,000 calendar years BP during the Bølling/Allerød (B/A) period. Our data synthesis suggests that biogenic fluxes were in general lowest during the last glacial period, increased somewhat in the Northwest Pacific during Heinrich Event 1, and reached a maximum across the entire North Pacific during the B/A period. We evaluate several mechanisms as possible drivers of deglacial change in biogenic fluxes in the North Pacific, including changes in preservation, sediment focusing, sea ice extent, iron inputs, stratification, and circulation shifts initiated in the North Atlantic and North Pacific. Our analysis suggests that while micronutrient sources likely contributed to some of the observed changes, the heterogeneity in timing of glaciogenic retreat and sea level make these mechanisms unlikely causes of region-wide contemporaneous peaks in export production. We argue that paleo-observations are most consistent with ventilation increases in both the North Pacific (during H1) and North Atlantic (during B/A) being the primary drivers of increases in biogenic flux during the deglaciation, as respectively they were likely to bring nutrients to the surface via increased vertical mixing and shoaling of the global thermocline.

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We compared the suitability of two skeletal materials of the Atlantic brain coral Diploria strigosa for 230Th/U-dating: the commonly used bulk material comprising all skeletal elements and the denser theca wall material. Eight fossil corals of presumably Last Interglacial age from Bonaire, southern Caribbean Sea, were investigated, and several sub-samples were dated from each coral. For four corals, both the ages and the activity ratios of the bulk material and theca wall agree within uncertainty. Three corals show significantly older ages for their bulk material than for their theca wall material as well as substantially elevated 232Th content and (230Th/238U) ratios. The bulk material samples of another coral show younger ages and lower (230Th/238U) ratios than the corresponding theca wall samples. This coral also contains a considerable amount of 232Th. The application of the available open-system models developed to account for post-depositional diagenetic effects in corals shows that none of the models can successfully be applied to the Bonaire corals. The most likely explanation for this observation is that the assumptions of the models are not fulfilled by our data set. Comparison of the theca wall and bulk material data enables us to obtain information about the open-system processes that affected the corals. The corals showing apparently older ages for their bulk material were probably affected by contamination with a secondary (detrital) phase. The most likely source of the detrital material is carbonate sand. The higher (230Th/232Th) ratio of this material implies that detrital contamination would have a much stronger impact on the ages than a contaminant with a bulk Earth (230Th/232Th) ratio and that the threshold for the commonly applied 232Th reliability criterion would be much lower than the generally used value of 1 ng g^-1. The coral showing apparently younger ages for its bulk material was probably influenced by more than one diagenetic process. A potential scenario is a combination of detrital contamination and U addition by secondary pore infillings. Our results show that the dense theca wall material of D. strigosa is generally less affected by post-depositional open-system behaviour and better suited for 230Th/U-dating than the bulk material. This is also obvious from the fact that all ages of theca wall material reflect a Last Interglacial origin (~125 ka), whereas the bulk material samples are either substantially older or younger. However, for some corals, the 230Th/U-ages and activity ratios of the bulk material and the theca wall samples are similar. This shows that strictly reliable 230Th/U-ages can also be obtained from bulk material samples of exceptionally well-preserved corals. However, the bulk material samples more frequently show elevated activity ratios and ages than the corresponding theca wall samples. Our findings should be generally applicable to brain corals (Mussidae) that are found in tropical oceans worldwide and may enable reliable 230Th/U-dating of fossil corals with similar skeletal architecture, even if their bulk skeleton is altered by diagenesis. The 230Th/U-ages we consider reliable (120-130 ka), along with a recently published age of 118 ka, provide the first comprehensive dating of the elevated lower reef terrace at Bonaire (118-130 ka), which is in agreement in timing and duration with other Last Interglacial records.