Radioactivity distribution in some Permian sediments from the Irati and Corumbatal formations of the Parana basin, southeastern Brazil

in the city of Limeira, southeastern Brazil, an important exposure of Permian sediments of the Parana basin was revealed by an open pit mine that exploits limestone for production of soil correction compounds and raw materials for the ceramic industry. The radioactivity of these sediments was investigated in some detail and the results provided a general view of the vertical distributions of uranium, thorium and potassium concentrations and of the element ratios U/K, U/Th and Th/K. In general, the concentrations of the main natural radioactive elements are low, with uranium being enriched in some limestone and shale levels. In addition the results showed that the U-238 series is in radioactive disequilibrium in many of the analyzed samples. Although the origin of the observed disequilibrium has not been investigated, the results suggest that it is due to weathering processes and water interaction with the rock matrix. (C) 2003 Elsevier Ltd. All rights reserved.

Implications of groundwater weathered profile interactions to the mobilization of radionuclides

This study reports the nature and extent of open-system interaction between groundwater and a weathered profile developed in the high grade thorium and REE ore body in Morro do Ferro, Pocos de Caldas plateau. The radioelement mobility in the shallow oxidizing environment was considered by using chemical data in conjunction with U-234/U-238, Ra-226/Th-230, Th-230/U-234, Th-228/Th-232, Ra-228/Th-232 and Th-230/Ra-228 activity ratios (AR's) for borehole spoil and groundwater samples.Recharging groundwater from the studied borehole has low salinity values, with total dissolved solids content of 14.7 mg/l and total ionic strength of 0.00018. The ratio of the weight of dissolved radioelement per unit volume of solution to the weight of radioelement in solid phase per unit weight of solid phase showed that the radioelement solubility in the studied waters varied according to the following order: radium> uranium >thorium.U-234/U-238 AR's less than 1 were measured in solid phase and can justify the enhancement of U-234 in solution. Ra-226/Th-230 AR's greater than 1 and Th-230/U-234 AR'S less than 1 were evaluated between 20 and 27 m in depth, where a 2.1-m thick magnetite dike was intersected. These ratios could be justified by deposition of U and Ra associated with Fe-Mn oxides and kaolinite, where mineral saturation indices evaluated from the available data confirm this possibility. Covariations among disequilibria involving Th-228/(228) Ra and Ra-228/Th-232 AR's showed the preferential removal of Ra-228 relative to Tn isotopes, Th-228 and Th-232. The recent deposition of radium within the timescale of at least the last 35 years also is suggested. (C) 1998 Elsevier B.V. Ltd. All rights reserved.

The natural radioactivity in Guarani aquifer groundwater, Brazil

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

Health risk related to radon in a thermal spa utilizing waters from Guarani aquifer

This investigation was carried out within the Parana sedimentary basin, Brazil, involved the sampling of groundwater and air, and was realized with the purpose of evaluating the radioactivity, due to radon gas, in a thermal spa utilizing the waters from Guarani (Botucatu-Piramboia) aquifer. The results reported here provide additional information relative to that of previous studies focusing on the presence of radionuclides in the aquifer, which have mainly characterized those belonging to uranium and thorium series decay, such as the uranium isotopes (U-238 and U-234), radium isotopes (Ra-226 and Ra-228), radon daughters (Bi-214 and Pb-214) and radon (Rn-222) itself the results obtained were compared with the maximum permissible concentration limits in air and drinking water defined by international standards, such as the guidelines for drinking water quality established by the World Health Organization. The possible processes responsible for the presence of radon in the aquifer were also considered in order to evaluate the data obtained.

Geo(anthropo)genic factors affecting the radioactivity in groundwaters from Guarani aquifer, Brazil

This investigation was carried out within the Paraná sedimentary basin, involved the sampling of 77 pumped tubular wells, and was realized with the puipose of evaluating the radioactivity in the Brazilian part of Guarani (Botucatu-Pirambóia, Tacuarembó, Misiones) aquifer. The radioactivity due to nuclides belonging to uranium and thorium series decay was investigated in terms of the uranium isotopes 234U and 238U, radon (222Rn), and the radium isotopes 226Ra and 228Ra. The obtained results were compared with the maximum permissible concentration limits in drinking water defined by the Brazilian national standard, as well with the guidelines for drinking water quality established by the World Health Organization. The importance of water-rock/soil interactions was considered in order to explain most of the obtained data.

Geochemical and radioactivity characterization of rocks from the Rio Preto (Go) Project

The Rio Preto Project, developed by the extinct Brazilian nuclear state company, Nuclebrás, during the late 70s and early 80s, consisted of basic geological mapping and radiometric characterization by aerogeophysical gamma-ray spectrometry, without channel discrimination, of a surface area of 650 km2 located to the west of the Chapada dos Veadeiros National Park on the northeastern of Goiás State, Brazil, including the confluence area of Claro and Preto Rivers. Additionally, the natural radioelements U, Th and 40K were determined by gamma-ray spectrometry in 300 rock samples from cores of the Rio Preto Project area. The tests were conducted at LABIDRO-Isotopes and Hydrochemistry Laboratory of the Departament of Petrology and Metallogeny (DPM) of the Institute of Geosciences and Exact Sciences, UNESP, in Rio Claro, SP, Brazil. This paper reports the results of petrographic characterization and chemical analyses of major oxides (SiO2, TiO2, Al2O3, Fe2O3, MgO, MnO, K2O, Na2O, CaO and P2O5) for all samples used to determine the natural radioelements present in the region. The organic matter content results obtained by colorimetry are also reported for selected cores of different lithotypes in order to investigate the possible relationship between graphite and the radioelements uranium and thorium. Finally, uranium content and 234U/238U activity ratio data for selected samples of schists and gneisses of the Lower Member of the Ticunzal Formation suggest the influence of weathering processes in the area. © 2012 Sociedade Brasileira de Geofísica.

Simulação de perfis nucleares de poço em formações complexas

A identificação e descrição dos caracteres litológicos de uma formação são indispensáveis à avaliação de formações complexas. Com este objetivo, tem sido sistematicamente usada a combinação de ferramentas nucleares em poços não-revestidos. Os perfis resultantes podem ser considerados como a interação entre duas fases distintas: • Fase de transporte da radiação desde a fonte até um ou mais detectores, através da formação. • Fase de detecção, que consiste na coleção da radiação, sua transformação em pulsos de corrente e, finalmente, na distribuição espectral destes pulsos. Visto que a presença do detector não afeta fortemente o resultado do transporte da radiação, cada fase pode ser simulada independentemente uma da outra, o que permite introduzir um novo tipo de modelamento que desacopla as duas fases. Neste trabalho, a resposta final é simulada combinando soluções numéricas do transporte com uma biblioteca de funções resposta do detector, para diferentes energias incidentes e para cada arranjo específico de fontes e detectores. O transporte da radiação é calculado através do algoritmo de elementos finitos (FEM), na forma de fluxo escalar 2½-D, proveniente da solução numérica da aproximação de difusão para multigrupos da equação de transporte de Boltzmann, no espaço de fase, dita aproximação P₁, onde a variável direção é expandida em termos dos polinômios ortogonais de Legendre. Isto determina a redução da dimensionalidade do problema, tornando-o mais compatível com o algoritmo FEM, onde o fluxo dependa exclusivamente da variável espacial e das propriedades físicas da formação. A função resposta do detector NaI(Tl) é obtida independentemente pelo método Monte Carlo (MC) em que a reconstrução da vida de uma partícula dentro do cristal cintilador é feita simulando, interação por interação, a posição, direção e energia das diferentes partículas, com a ajuda de números aleatórios aos quais estão associados leis de probabilidades adequadas. Os possíveis tipos de interação (Rayleigh, Efeito fotoelétrico, Compton e Produção de pares) são determinados similarmente. Completa-se a simulação quando as funções resposta do detector são convolvidas com o fluxo escalar, produzindo como resposta final, o espectro de altura de pulso do sistema modelado. Neste espectro serão selecionados conjuntos de canais denominados janelas de detecção. As taxas de contagens em cada janela apresentam dependências diferenciadas sobre a densidade eletrônica e a fitologia. Isto permite utilizar a combinação dessas janelas na determinação da densidade e do fator de absorção fotoelétrico das formações. De acordo com a metodologia desenvolvida, os perfis, tanto em modelos de camadas espessas quanto finas, puderam ser simulados. O desempenho do método foi testado em formações complexas, principalmente naquelas em que a presença de minerais de argila, feldspato e mica, produziram efeitos consideráveis capazes de perturbar a resposta final das ferramentas. Os resultados mostraram que as formações com densidade entre 1.8 e 4.0 g/cm³ e fatores de absorção fotoelétrico no intervalo de 1.5 a 5 barns/e^-, tiveram seus caracteres físicos e litológicos perfeitamente identificados. As concentrações de Potássio, Urânio e Tório, puderam ser obtidas com a introdução de um novo sistema de calibração, capaz de corrigir os efeitos devidos à influência de altas variâncias e de correlações negativas, observadas principalmente no cálculo das concentrações em massa de Urânio e Potássio. Na simulação da resposta da sonda CNL, utilizando o algoritmo de regressão polinomial de Tittle, foi verificado que, devido à resolução vertical limitada por ela apresentada, as camadas com espessuras inferiores ao espaçamento fonte - detector mais distante tiveram os valores de porosidade aparente medidos erroneamente. Isto deve-se ao fato do algoritmo de Tittle aplicar-se exclusivamente a camadas espessas. Em virtude desse erro, foi desenvolvido um método que leva em conta um fator de contribuição determinado pela área relativa de cada camada dentro da zona de máxima informação. Assim, a porosidade de cada ponto em subsuperfície pôde ser determinada convolvendo estes fatores com os índices de porosidade locais, porém supondo cada camada suficientemente espessa a fim de adequar-se ao algoritmo de Tittle. Por fim, as limitações adicionais impostas pela presença de minerais perturbadores, foram resolvidas supondo a formação como que composta por um mineral base totalmente saturada com água, sendo os componentes restantes considerados perturbações sobre este caso base. Estes resultados permitem calcular perfis sintéticos de poço, que poderão ser utilizados em esquemas de inversão com o objetivo de obter uma avaliação quantitativa mais detalhada de formações complexas.

Continental degassing of He-4 by surficial discharge of deep groundwater

Radiogenic He-4 is produced by the decay of uranium and thorium in the Earths mantle and crust. From here, it is degassed to the atmosphere(1-5) and eventually escapes to space(1,5,6). Assuming that all of the He-4 produced is degassed, about 70% of the total He-4 degassed from Earth comes from the continental crust(2,-5,7). However, the outgoing flux of crustal He-4 has not been directly measured at the Earths surface(2) and the migration pathways are poorly understood(2-4,7,8). Here we present measurements of helium isotopes and the long-lived cosmogenic radio-isotope Kr-81 in the deep, continental-scale Guarani aquifer in Brazil and show that crustal He-4 reaches the atmosphere primarily by the surficial discharge of deep groundwater. We estimate that He-4 in Guarani groundwater discharge accounts for about 20% of the assumed global flux from continental crust, and that other large aquifers may account for about 33%. Old groundwater ages suggest that He-4 in the Guarani aquifer accumulates over half- to one-million-year timescales. We conclude that He-4 degassing from the continents is regulated by groundwater discharge, rather than episodic tectonic events, and suggest that the assumed steady state between crustal production and degassing of He-4, and its resulting atmospheric residence time, should be re-examined.

Discovery and cross-section measurement of neutron-rich isotopes in the element range from neodymium to platinum with the FRS

Using the high-resolution performance of the fragment separator FRS at GSI we have discovered 60 new neutron-rich isotopes in the atomic number range of 60 <= Z <= 78. The new isotopes were unambiguously identified in reactions with a U-238 beam impinging on a Be target at 1 GeV/nucleon. The production cross-section for the new isotopes have been measured down to the pico-barn level and compared with predictions of different model calculations. For elements above hafnium fragmentation is the dominant reaction mechanism which creates the new isotopes, whereas fission plays a dominant role for the production of the new isotopes up to thulium. (C) 2012 Elsevier B.V. All rights reserved.

Bestimmung der Ionisationsenergie von Actinium und Ultraspurenanalyse von Plutonium mit resonanter Ionisationsmassenspektrometrie (RIMS)

ZusammenfassungDie Resonanzionisationsmassenspektrometrie (RIMS) verbindet hohe Elementselektivität mit guter Nachweiseffizienz. Aufgrund dieser Eigenschaften ist die Methode für Ultraspurenanalyse und Untersuchungen an seltenen oder schwer handhabbaren Elementen gut geeignet. Für RIMS werden neutrale Atome mit monochromatischem Laserlicht ein- oder mehrfach resonant auf energetisch hoch liegende Niveaus angeregt und anschließend durch einen weiteren Laserstrahl oder durch ein elektrisches Feld ionisiert. Die Photoionen werden in einem Massenspektrometer massenselektiv registriert.Ein Beispiel für die Anwendung von RIMS ist die präzise Bestimmung der Ionisationsenergie als fundamentale physikalisch-chemische Eigenschaft eines bestimmten Elements; insbesondere bei den Actinoiden ist die Kenntnis der Ionisationsenergie von Interesse, da es dort bis zur Anwendung der laser-massenspektroskopischer Methode nur wenige experimentelle Daten gab. Die Bestimmung der Ionisationsenergie erfolgt durch die Methode der Photoionisation im elektrischen Feld gemäß dem klassischen Sattelpunktsmodell. Im Experiment werden neutrale Atome in einem Atomstrahl mittels Laserlicht zunächst resonant angeregt. Die angeregten Atome befinden sich in einem äußeren, statischen elektrischen Feld und werden durch einen weiteren Laserstrahl, dessen Wellenlänge durchgestimmt wird, ionisiert. Das Überschreiten der Laserschwelle macht sich durch einen starken Anstieg im Ionensignal bemerkbar. Man führt diese Messung bei verschiedenen elektrischen Feldstärken durch und erhält bei Auftragen der Ionisationsschwellen gegen die Wurzel der elektrischen Feldstärke durch Extrapolation auf die Feldstärke Null die Ionisationsenergie.Im Rahmen dieser Arbeit wurde die Ionisationsenergie von Actinium erstmalig zu 43398(3) cm-1 º 5,3807(4) eV experimentell bestimmt. Dazu wurden Actiniumatome zunächst einstufig resonant mit einem Laser mit einer Wellenlänge von 388,67 nm auf einen Zustand bei 25729,03 cm-1 angeregt und anschließend mit Laserlicht mit einer Wellenlänge von ca. 568 nm ionisiert. Damit sind die Ionisationsenergien aller Actinoiden bis einschließlich Einsteinium mit Ausnahme von Protactinium bekannt. Als Atomstrahlquelle wird ein spezielles 'Sandwichfilament' benutzt, bei dem das Actinoid als Hydroxid auf eine Tantalfolie aufgebracht und mit einer reduzierenden Deckschicht überzogen wird. Das Actinoid dampft bei Heizen dieser Anordnung atomar ab. Bei den schwereren Actinoiden wurde Titan als Deckschicht verwendet. Um einen Actiniumatomstrahl zu erzeugen, wurde aufgrund der hohen Abdampftemperaturen statt Titan erstmals Zirkonium eingesetzt. Bei Protactinium wurde Thorium, welches noch stärkere Reduktionseigenschaften aufweist, als Deckmaterial eingesetzt. Trotzdem gelang es mit der 'Sandwichtechnik' nicht, einen Protactiniumatomstrahl zu erzeugen. In der Flugzeitapparatur wurde lediglich ein Protactinium-monoxidionensignal detektiert. Um ein erst seit kurzem verfügbares Fest-körperlasersystem zu explorieren, wurden zusätzlich noch die bekannten Ionisations-ener-gien von Gadolinium und Plutonium erneut bestimmt. Die gemessenen Werte stimmen mit Literaturdaten gut überein.Ferner wurde noch ein bestehender Trennungsgang für Plutonium aus Umweltproben auf die Matrices Meerwasser und Hausstaub angepasst und für die Bestimmung von Plutonium und dessen Isotopenzusammensetzung in verschiedenen Probenreihen mittels RIMS eingesetzt. Der modifizierte Trennungsgang ermöglicht das schnelle Aufarbeiten von großen Probenmengen für Reihenuntersuchungen von Plutoniumkontaminationen. Die ermittelten Gehalten an 239Pu lagen zwischen 8,2*107 Atome pro 10 l Meerwasserprobe und 1,7*109Atome pro Gramm Staubprobe.

Astrophysikalische Bedingungen für einen r-Prozess im Hoch-Entropie-Wind von Typ II Supernovae

Sterne mit einer Anfangsmasse zwischen etwa 8 und 25 Sonnenmassen enden ihre Existenz mit einer gewaltigen Explosion, einer Typ II Supernova. Die hierbei entstehende Hoch-Entropie-Blase ist ein Bereich am Rande des sich bildenden Neutronensterns und gilt als möglicher Ort für den r-Prozess. Wegen der hohen Temperatur T innerhalb der Blase ist die Materie dort vollkommen photodesintegriert. Das Verhältnis von Neutronen zu Protonen wird durch die Elektronenhäufigkeit Ye beschrieben. Die thermodynamische Entwicklung des Systems wird durch die Entropie S gegeben. Da die Expansion der Blase schnell vonstatten geht, kann sie als adiabatisch betrachtet werden. Die Entropie S ist dann proportional zu T^3/rho, wobei rho die Dichte darstellt. Die explizite Zeitentwicklung von T und rho sowie die Prozessdauer hängen von Vexp, der Expansionsgeschwindigkeit der Blase, ab. Der erste Teil dieser Dissertation beschäftigt sich mit dem Prozess der Reaktionen mit geladenen Teilchen, dem alpha-Prozess. Dieser Prozess endet bei Temperaturen von etwa 3 mal 10^9 K, dem sogenannten "alpha-reichen" Freezeout, wobei überwiegend alpha-Teilchen, freie Neutronen sowie ein kleiner Anteil von mittelschweren "Saat"-Kernen im Massenbereich um A=100 gebildet werden. Das Verhältnis von freien Neutronen zu Saatkernen Yn/Yseed ist entscheidend für den möglichen Ablauf eines r-Prozesses. Der zweite Teil dieser Arbeit beschäftigt sich mit dem eigentlichen r-Prozess, der bei Neutronenanzahldichten von bis zu 10^27 Neutronen pro cm^3 stattfindet, und innerhalb von maximal 400 ms sehr neutronenreiche "Progenitor"-Isotope von Elementen bis zum Thorium und Uran bildet. Bei dem sich anschliessendem Ausfrieren der Neutroneneinfangreaktionen bei 10^9 K und 10^20 Neutronen pro cm^3 erfolgt dann der beta-Rückzerfall der ursprünglichen r-Prozesskerne zum Tal der Stabilität. Diese Nicht-Gleichgewichts-Phase wird in der vorliegenden Arbeit in einer Parameterstudie eingehend untersucht. Abschliessend werden astrophysikalische Bedingungen definiert, unter denen die gesamte Verteilung der solaren r-Prozess-Isotopenhäufigkeiten reproduziert werden können.

Spurenanalyse von Aktiniden in der Umwelt mittels Resonanzionisations-Massenspektrometrie

In dieser Arbeit wurde die Methode der resonanten Ionisation von neutralen Atomen mittels Laserstrahlung auf die leichten Aktinide Thorium, Uran, Neptunium und Plutonium angewendet und für die Ultraspurenanalyse optimiert. Der empfindliche Nachweis dieser Aktinide stellt eine Herausforderung für die Beobachtung und Bestimmung von radioaktiven Verunreinigungen aus kerntechnischen Anlagen in der Umwelt dar. In einem für diese Untersuchungen entwickelten Quadrupolmassenspektrometer konnte durch Resonanzionisationsspektroskopie jeweils eine Reihe unbekannter Energiezustände in der Elektronenhülle des neutralen Atoms der oben genannten Aktinide identifiziert, sowie effiziente Anregungsschemata für die resonante Ionisation entwickelt und charakterisiert werden. Durch die verwendete in-source-Ionisation, die aufgrund der guten Überlagerung von Laserstrahlung und Atomstrahl eine hohe Nachweiseffizienz gewährleistet, konnten diese Untersuchungen bereits mit einem, für Radionuklide notwendigen, geringen Probeneintrag erfolgen. Die resonante Ionisation erlaubt durch die selektiven resonanten Prozesse eine Unterdrückung unerwünschter Kontaminationen und wurde auf den analytischen Nachweis von Ultraspurengehalten in Umweltproben, sowie die Bestimmung der entsprechenden Isotopenzusammensetzung optimiert. Durch die effiziente in-source-Ionisation mit leistungsstarker gepulster Laserstrahlung, konnten Nachweiseffizienzen im Bereich von bis zu 1% erreicht werden. Dabei wurden für Plutonium in synthetischen Proben, aber auch in ersten Umweltproben, Nachweisgrenzen von 10^4-10^5 Atomen erzielt. Die Verwendung spektral schmalbandiger Dauerstrichlaser und eine Ionisation transversal zum frei propagierenden Atomstrahl ermöglicht durch Auflösung der Isotopieverschiebung eine hohe Selektivität gegenüber dominanten Nachbarisotopen, wohingegen die Ionisationseffizienz deutlich abnimmt. Hiermit konnte für das Ultraspurenisotop U-236 eine Nachweisgrenze bis hinab zu 10^-9 für das Isotopenverhältnis N(U-236)/N(U-238) bestimmt werden.

Continental degassing of 4He by surficial discharge of deep groundwater

Radiogenic He is produced by the decay of uranium and thorium in the Earth’s mantle and crust. From here, it is degassed to the atmosphere and eventually escapes to space. Assuming that all of the 4He produced is degassed, about 70% of the total He degassed from Earth comes from the continental crust. However, the outgoing flux of crustal He has not been directly measured at the Earth’s surface and the migration pathways are poorly understood. Here we present measurements of helium isotopes and the long-lived cosmogenic radio-isotope Kr in the deep, continental-scale Guarani aquifer in Brazil and show that crustal He reaches the atmosphere primarily by the surficial discharge of deep groundwater. We estimate that He in Guarani groundwater discharge accounts for about 20% of the assumed global flux from continental crust, and that other large aquifers may account for about 33%. Old groundwater ages suggest that He in the Guarani aquifer accumulates over half- to one-millionyear timescales. We conclude that He degassing from the continents is regulated by groundwater discharge, rather than episodic tectonic events, and suggest that the assumed steady state between crustal production and degassing of He, and its resulting atmospheric residence time, should be re-examined.

Imaging the South Pole-Aitken basin in backscattered neutral hydrogen atoms

The lunar surface is very efficient in reflecting impinging solar wind ions as energetic neutral atoms (ENAs). A global analysis of lunar hydrogen ENAs showed that on average 16% of the solar wind protons are reflected, and that the reflected fraction can range from less than 8% to more than 24%, depending on location. It is established that magnetic anomalies reduce the flux of backscattered hydrogen ENAs by screening-off a fraction of the impinging solar wind. The effects of the surface properties, such as porosity, roughness, chemical composition, and extent of weathering, were not known. In this paper, we conduct an in-depth analysis of ENA observations of the South Pole-Aitken basin to determine which of the surface properties might be responsible for the observed variation in the integral ENA flux. The South Pole-Aitken basin with its highly variable surface properties is an ideal object for such studies. It is very deep, possesses strikingly elevated concentrations in iron and thorium, has a low albedo and coincides with a cluster of strong magnetic anomalies located on the northern rim of the basin. Our analysis shows that whereas, as expected, the magnetic anomalies can account well for the observed ENA depletion at the South Pole-Aitken basin, none of the other surface properties seem to influence the ENA reflection efficiency. Therefore, the integral flux of backscattered hydrogen ENAs is mainly determined by the impinging plasma flux and ENA imaging of backscattered hydrogen captures the electrodynamics of the plasma at the surface. We cannot exclude minor effects by surface features. (C) 2015 Elsevier Ltd. All rights reserved.