This thesis contains an account of a measurement of the neutron energy spectrum from radiative pion capture in carbon, oxygen and calcium. The measurement was performed at six n-γ correlation angles for the case of carbon and oxygen, and seven n-γ correlation angles for the case of calcium. The observed energy spectra fall off approximately exponentially between 2 and 30 MeV. Evidence of resonance structure was observed at about 4 MeV in the energy spectra of carbon and oxygen. This is in agreement with a theoretical prediction of the giant multipole excitation model. The neutron yield versus n-γ correlation angles peaks at 180° for all three nuclei studied. This indicates the quasi-free mechanism also plays an important role in the radiative pion capture process. / Ph. D.

In this thesis, we study low energy capture reactions and neutron-deuteron elastic scattering using halo effective field theory (EFT). At low energy, EFT provides a general framework to analyze physical systems regarding as an expansion of short-distance over large distance scales. We provide a model-independent calculation for neutron capture on carbon-14, radiative capture of 3He-4He, radiative capture of 3H-4He, and neutrondeuteron (n-d) doublet channel elastic scattering using halo EFT. These reactions play a significant role in the carbon-nitrogen-oxygen (CNO) cycle, solar neutrino flux measurement, lithium production, and big bang nucleosynthesis (BBN) in the early universe. The cross section is calculated for radiative neutron capture in carbon-14 using halo EFT. This reaction is slowest in the CNO cycle, and it acts as a bottleneck in the production of heavier nuclei A greater than 14. The capture contribution is different from Brett-Wigner resonance because of interference between resonant and non-resonant contribution. Also, we calculated, electromagnetic form factors for one-neutron halo nuclei such as carbon-15, beryllium-11, and carbon-19 using EFT. The electromagnetic form factors depend on the nucleon separation energy, effective range, and the two-body current. The EFT expressions are presented to leading order (LO) for 15C and next-to-leading order (NLO) for 11Be and 19C. We also calculated astronomical Sactor for 3He-4He and 3H-4He radiative capture reactions. The low energy Sactor for these reactions are important to understand the Li problem and neutrino physics. At the LO, the capture amplitude contains the initial state swave strong and Coulomb interactions summed to all orders. The NLO contribution comes from non-perturbative Coulomb interaction. Our calculated astrophysical Sactor for 3He- 4He is slightly above the average compared to the other measurement and prediction but consistent within current error bars. The Sactor for 3H-4He is also compatible with the experimental extrapolation. Finally, we studied doublet channel n-d scattering using halo EFT. A two dimer halo EFT is developed to describe the virtual state and three-body bound state in n-d scattering. We show the connection between virtual state and three-body bound state using S-matrix analysis and phase shift analysis which is supported by the Efimov plots.

No description available.

No description available.

Este trabalho apresenta e consolida uma metodologia alternativa para a determinação de taxas de reação nuclear ao longo da direção radial das pastilhas combustíveis sem necessidade de intensos fluxos neutrônicos. Esta técnica se baseia na irradiação de um disco de UO2 inserido no interior de uma vareta combustível desmontável no núcleo do reator IPEN/MB-01. Após a irradiação são realizadas várias espectrometrias gama do disco utilizando um detector HPGe alternando sequencialmente 6 colimadores de chumbo com diâmetros diferentes. Consequentemente, as reações nucleares de captura radiativa que ocorrem nos átomos de 238U, juntamente com as fissões que ocorrem em ambos 235U e 238U são mensuradas em função de 6 regiões radiais distintas do disco combustível. As correções de eficiência geométrica devido à introdução dos colimadores no sistema de detecção HPGe são determinadas através do código MCNP-5. As medidas de taxa de fissão são realizadas utilizando o 99Mo como radionuclídeo traçador. Esse radionuclídeo foi estudado e provou-se ideal para estas medidas por possuir um comportamento linear de formação, alto rendimento de fissão e principalmente por emitir fótons de baixa energia. As medidas foram efetuadas irradiando discos de UO2 (com enriquecimento de 4,3%) na posição central do reator IPEN/MB-01 a potência de 100 Watts durante uma hora. Algumas medidas foram realizadas utilizando uma luva de cádmio envolta na vareta combustível para determinar as taxas de reação nuclear na faixa de energia epitérmica. Os resultados experimentais obtidos são comparados a cálculos de taxa de reação nuclear via MCNP-5 utilizando a biblioteca de dados ENDF/B-VII.0, os quais apresentaram discrepâncias de no máximo 9% para as taxas de captura no 238U e 14% para as taxas de fissão no U na faixa epitérmica. Foram obtidos valores máximos de 4,5% para incertezas relativas as taxas de captura total e epitérmica e para as taxas de fissão total e epitérmica valores máximos de 11,3%. / This research presents and consolidates an alternative methodology for determining nuclear reaction rates along the radial direction of the fuel pellets which does not require high neutron flux. This technique is based on irradiating a thin UO2 disk inserted into a removable fuel rod at the IPEN/MB-01 reactor core. Several gamma spectrometries are performed after irradiation using a HPGe detector. Six lead collimators with different diameters are sequentially alternated during this process, thus, the nuclear radioactive capture which occurs in 238U and the fissions which occur in both 235U and 238U are measured according to six different radial regions of the fuel disk. Geometric efficiency corrections due to the introduction of collimators in HPGe detection system are determined by MCNP-5 code. The fission rate measurements are performed using the 99Mo. This radionuclide was studied and proved ideal for these measurements because it is formed in linear behavior in the reactor core, have a high yield fission and emits low-energy photons. Measurements were performed irradiating UO2 disks (with 4.3% enrichment) in the central position of the IPEN/MB-01 core at 100 watts power level during one hour. Some measurements were performed using a cadmium glove wrapped in the fuel rod to determine the nuclear reaction rates in the epithermal energy range. The experimental results obtained are compared with nuclear reaction rate calculations by means of MCNP-5 with ENDF/B-VII.0 data library showing discrepancies of up to 9% in 238U capture rates and 14% for U fission rates for epithermal energies. Uncertainties regarding the nuclear capture rates have maximum values of 4.5% and the fission rates has maximum values of 11.3%.

Este trabalho apresenta e consolida uma metodologia alternativa para a determinação de taxas de reação nuclear ao longo da direção radial das pastilhas combustíveis sem necessidade de intensos fluxos neutrônicos. Esta técnica se baseia na irradiação de um disco de UO2 inserido no interior de uma vareta combustível desmontável no núcleo do reator IPEN/MB-01. Após a irradiação são realizadas várias espectrometrias gama do disco utilizando um detector HPGe alternando sequencialmente 6 colimadores de chumbo com diâmetros diferentes. Consequentemente, as reações nucleares de captura radiativa que ocorrem nos átomos de 238U, juntamente com as fissões que ocorrem em ambos 235U e 238U são mensuradas em função de 6 regiões radiais distintas do disco combustível. As correções de eficiência geométrica devido à introdução dos colimadores no sistema de detecção HPGe são determinadas através do código MCNP-5. As medidas de taxa de fissão são realizadas utilizando o 99Mo como radionuclídeo traçador. Esse radionuclídeo foi estudado e provou-se ideal para estas medidas por possuir um comportamento linear de formação, alto rendimento de fissão e principalmente por emitir fótons de baixa energia. As medidas foram efetuadas irradiando discos de UO2 (com enriquecimento de 4,3%) na posição central do reator IPEN/MB-01 a potência de 100 Watts durante uma hora. Algumas medidas foram realizadas utilizando uma luva de cádmio envolta na vareta combustível para determinar as taxas de reação nuclear na faixa de energia epitérmica. Os resultados experimentais obtidos são comparados a cálculos de taxa de reação nuclear via MCNP-5 utilizando a biblioteca de dados ENDF/B-VII.0, os quais apresentaram discrepâncias de no máximo 9% para as taxas de captura no 238U e 14% para as taxas de fissão no U na faixa epitérmica. Foram obtidos valores máximos de 4,5% para incertezas relativas as taxas de captura total e epitérmica e para as taxas de fissão total e epitérmica valores máximos de 11,3%. / This research presents and consolidates an alternative methodology for determining nuclear reaction rates along the radial direction of the fuel pellets which does not require high neutron flux. This technique is based on irradiating a thin UO2 disk inserted into a removable fuel rod at the IPEN/MB-01 reactor core. Several gamma spectrometries are performed after irradiation using a HPGe detector. Six lead collimators with different diameters are sequentially alternated during this process, thus, the nuclear radioactive capture which occurs in 238U and the fissions which occur in both 235U and 238U are measured according to six different radial regions of the fuel disk. Geometric efficiency corrections due to the introduction of collimators in HPGe detection system are determined by MCNP-5 code. The fission rate measurements are performed using the 99Mo. This radionuclide was studied and proved ideal for these measurements because it is formed in linear behavior in the reactor core, have a high yield fission and emits low-energy photons. Measurements were performed irradiating UO2 disks (with 4.3% enrichment) in the central position of the IPEN/MB-01 core at 100 watts power level during one hour. Some measurements were performed using a cadmium glove wrapped in the fuel rod to determine the nuclear reaction rates in the epithermal energy range. The experimental results obtained are compared with nuclear reaction rate calculations by means of MCNP-5 with ENDF/B-VII.0 data library showing discrepancies of up to 9% in 238U capture rates and 14% for U fission rates for epithermal energies. Uncertainties regarding the nuclear capture rates have maximum values of 4.5% and the fission rates has maximum values of 11.3%.

Des calculs de type modèle en couches ont été réalisés dans un espace de valence 1¯hω complet pour les noyaux de la couche sd. Ces calculs ont permis pour la première fois de prédire la durée de vie des états de parité positive et négative des noyaux riches en neutrons de la couche sd. Les durées de vie prédites (1 - 100 ps) sont mesurables par la méthode de décalage Doppler différentiel.Le démonstrateur du détecteur γ européen de nouvelle génération, AGATA, en coïncidence avec le spectromètre magnétique PRISMA du LNL (Italie) et le plunger de l’Université de Cologne ont été utilisés pour mesurer les durées de vie des états excités dans 32,33Si et 35,36S. Les structures plus complexes, à n¯hω ont également été étudiées dans le 28Si. Ce dernier est un noyau important pour comprendre la compétition entre les structures de type champ moyen et les structures en agrégats. La réaction résonante de capture radiative d’ions lourds-légers 12C+16O a été réalisée à des énergies sous-coulombiennes. La décroissance γ complète depuis les résonances peuplées par laréaction jusqu’au niveau fondamental de 28Si a été mesurée pour la première fois à ces énergies et montre une forte alimentation d’états intermédiaires autour de 10 MeV. Les comparaisons avec des études de captures radiatives au-dessus de la barrière de Coulomb ont été effectuées et les résultats ont été interprétés en termes de l’alimentation favorisée d’états à isospin T = 1 dans le noyau autoconjugué 28Si. / New large-scale shell-model calculations with full 1¯hω valence space for the sd-nuclei has been used for the first time to predict lifetimes of positive and negative parity states in neutron rich Si isotopes. The predicted lifetimes (1 - 100 ps) fall in the range of the differential Doppler shift method. Using the demonstrator of the European next generation γ-ray array, AGATA, in coincidence with the large acceptance PRISMA magnetic spectrometer from LNL (Legnaro) and the differential plunger of the University of Cologne, lifetimes of excited states in 32,33Si and 35,36S nuclei were measured. In a second step, the n¯hω structure in the stable 28Si nucleus was also studied. 28Si is an important nucleus to understand the competition between mean-field and cluster structures. It displays a wealth of structures in terms of deformation and clustering. Light heavy-ion resonant radiative capture 12C+16O has been performed at energies below the Coulomb barrier. The measured γ-spectra indicate for the first time at these energies that the strongest part of the resonance decay proceeds though intermediate states around 10 MeV. Comparisons with previous radiative capture studies above the Coulomb barrier have been performed and the results have been interpreted in terms of a favoured feeding of T = 1 states in the 28Si self-conjugate nucleus.

The 14N(p,gamma)15O reaction is the slowest stage of the carbon-nitrogen-oxygen cycle of hydrogen burning and thus determines its reaction rate. Precise knowledge of its rate is required to improve the model of hydrogen burning in our sun. The reaction rate is a necessary ingredient for a possible solution of the solar abundance problem that led to discrepancies between predictions of the solar standard model and helioseismology. The solar 13N and 15O neutrino fluxes are used as independent observables that probe the carbon and nitrogen abundances in the solar core. This could settle the disagreement, if the 14N(p,gamma)15O reaction rate is known with high precision. After a review of several measurements its cross section was revised downward due to a much lower contribution by one particular transition, capture to the ground state in 15O. The evaluated total relative uncertainty is still 7.5%, in part due to an unsatisfactory knowledge of the excitation function over a wide energy range. The present work reports experimentally determined cross sections as astrophysical S-factor data at twelve energies between 0.357 - 1.292 MeV for the strongest transition, capture to the 6.79 MeV excited state in 15O with lower uncertainties than before and at ten energies between 0.479 - 1.202 MeV for the second strongest transition, capture to the ground state in 15O. In addition, an R-matrix fit is performed to estimate the impact of the new data on the astrophysical relevant energy range. The recently suggested slight S-factor enhancement at the Gamow window could not be confirmed and differences to previous measurements at energies around 1 MeV were observed. The present extrapolated zero-energy S-factors are S_6.79(0) = (1.19+-0.10) keV b and S_GS(0) = (0.25+-0.05) keV b and they are within the uncertainties consistent with values recommended by the latest review. / Die 14N(p,gamma)15O Reaktion ist die langsamste Phase im Bethe-Weizsäcker-Zyklus des Wasserstoffbrennens und bestimmt deshalb die Reaktionsrate des gesamten Zyklus. Präzise Werte für die Reaktionsrate sind notwendig um das Wasserstoffbrennen in unserer Sonne besser zu verstehen. Besonders das Problem widersprüchlicher Ergebnisse aus Vorhersagen des aktuellen Sonnenmodells und helioseismologischen Experimenten könnte durch genauer bekannte 14N(p,gamma)15O Reaktionsraten aufgelöst werden. Dafür soll der solare 13N und 15O Neutrinofluss von den beta+-Zerfällen als direkter Informationsträger über die Häufigkeit von Stickstoff und Kohlenstoff im Sonneninneren genutzt werden. Der für die Berechnung der Häufigkeiten benötigte Wirkungsquerschnitt der 14N(p,gamma)15O Reaktion wurde in einer Evaluation verschiedener Messungen reduziert, da der Anteil des direkten Protoneneinfang mit Übergang in den Grundzustand deutlich weniger zum gesamten Wirkungsquerschnitt beiträgt als zuvor angenommen. Die evaluierte relative Gesamtunsicherheit ist mit 7.5% dennoch hoch, was zu einem großen Teil an ungenügendem Wissen über die Anregungsfunktion in einem weiten Energiebereich liegt. In der vorliegenden Arbeit werden experimentell ermittelte Wirkungsquerschnitte in Form von astrophysikalischen S-Faktoren für zwei Übergänge vorgestellt. Für den stärksten Übergang, den Protoneneinfang zum angeregten Zustand bei 6.79 MeV in 15O, wurden zwölf S-Faktoren bei Energien zwischen 0.357 – 1.292 MeV mit geringeren Unsicherheiten als zuvor ermittelt und für den direkten Übergang in den Grundzustand zehn Werte zwischen 0.479 – 1.202 MeV. Außerdem wurde ein R-Matrix Fit durchgeführt um den Einfluss der neuen Daten auf Extrapolationen zum astrophysikalisch relevanten Energiebereich zu prüfen. Die kürzlich vorgeschlagene Erhöhung des S-Faktors im Gamow-Fenster konnte nicht bestätigt werden und es wurden auch Unterschiede zu bisherigen Messungen im Energiebereich um 1 MeV deutlich. Die neuen extrapolierten S-Faktoren sind S679(0) = (1.19±0.10) keV b und SGS(0) = (0.25 ± 0.05) keV b und sie stimmen mit den von der Evaluation empfohlenen Werten im Rahmen ihrer Unsicherheiten überein.

For several decades, the idea of flying and landing a less-than-man-rated nuclear reactor for planetary surface applications has been considered. This approach promises significant mass savings and therefore reduction in launch cost. To compensate for the lack of shielding, it has been suggested the use of in-situ materials for providing radiation protection. This would take the form of either raw dirt walls or processed soil materials into blocks or tile elements. As a first step in determining the suitability of this approach, it is necessary to understand the neutron activation characteristics of these soils. A simple assessment of these activation characteristics was conducted for both Martian and Lunar soils using ORIGEN2.2. An average composition for these soils was assumed. As a baseline material, commonly used NBS-03 concrete was compared against the soils. Preliminary results indicate that over 2.5 times more gamma-radiation production of these soils vs. concrete took place during the irradiation phase (a baseline of 2.4 x 1011 neutrons/sec-cm2 was assumed). This was due primarily to radiative capture on Na23 and Mn55 and subsequent decay of their activation products. This is does not necessarily disqualify these materials as potential shielding material since the -radiation output was only in the order of 4.2 x 108 photons/cm3-sec. Furthermore, these soils did not show any significant activity after shutdown of the neutron source (the reactor), since all activation products had very short half lives. Their performance in this area was comparable to that of NBS-03 concrete. / text

Les activités nucléaires génèrent des déchets radioactifs classés selon leur niveau d’activité et la durée de vie des radioéléments présents. La garantie d’un classement et d’une gestion optimale nécessite une caractérisation précise. Les déchets de moyenne et haute activité, contenant des radioéléments à vie très longue, seront stockés en profondeur pendant plusieurs centaines de milliers d’années, à l’issue desquelles il est nécessaire de pouvoir garantir l’absence de risques pour l’homme et l’environnement, non seulement sur le plan radiologique, mais aussi en ce qui concerne des éléments stables, toxiques du point de vue chimique. Cette thèse concerne la caractérisation par activation neutronique de ces éléments toxiques, ainsi que celle des matières nucléaires présentes dans les colis. Elle a été réalisée dans le cadre d’une collaboration entre le Laboratoire de Mesures Nucléaires du CEA Cadarache, en France, et l’institut de Gestion des Déchets Radioactifs et de Sûreté des Réacteurs du centre de recherche FZJ (Forschungszentrum Jülich), en Allemagne. La première étude a consisté à valider le modèle numérique de la cellule d’activation neutronique MEDINA (FZJ) avec le code de transport Monte Carlo MCNP. Les rayonnements gamma prompts de capture radiative d’échantillons contenant des éléments d’intérêt (béryllium, aluminium, chlore, cuivre, sélénium, strontium et tantale) ont été mesurés et comparés aux simulations avec diverses bases de données nucléaires, permettant d’aboutir à un accord satisfaisant et validant le schéma de calcul en vue des études suivantes. Ensuite, la mesure des rayonnements gamma retardés de fissions induites sur les isotopes 235U et 239Pu a été étudiée pour des fûts de 225 L contenant des enrobés bitumineux ou une matrice béton, représentatifs de déchets produits en France et en Allemagne. Les rendements d’émission des rayonnements gamma retardés de fission d’intérêt, cohérents avec ceux publiés dans la littérature, ont été déterminés à partir des mesures d’échantillons métalliques d’uranium et de plutonium dans la cellule d’activation neutronique REGAIN du LMN. Le signal utile a ensuite été extrapolé par simulation MCNP pour une répartition homogène d’isotopes 239Pu ou 235U dans les matrices considérées, en utilisant le modèle numérique de MEDINA. Des signaux faibles, de l’ordre de 100 coups par gramme d’isotope 239Pu ou 235U, ont été obtenus. Pour le colis d’enrobés bitumineux, le niveau d’irradiation gamma très élevé, dû à une activité en 137Cs de l’ordre de 1 TBq par fût, nécessiterait l’utilisation d’une collimation et/ou d’écrans pour éviter la saturation de l’électronique de mesure, rendant indétectables les rayonnements gamma retardés de fission. Les colis de déchets bétonnés produits en Allemagne présentant un niveau d’activité plus faible, il a été possible d’estimer des limites de détection allant de 10 à 290 g d’isotope fissile 235U ou 239Pu, selon la raie gamma considérée, suite à la mesure du bruit de fond actif dans MEDINA avec une matrice béton maquette. Afin d’améliorer ces performances, le blindage du détecteur germanium de MEDINA a été optimisé à l’aide de simulations MCNP, montrant la possibilité de réduire les bruits de fond gamma et neutron d’un facteur 4 et 5, respectivement. La validation expérimentale de l’efficacité du blindage a été effectuée à partir de configuration simples à implémenter dans MEDINA, confirmant les facteurs de réduction attendus. Un blindage du détecteur optimal permettrait d’améliorer les limites de détection et aussi d’utiliser une source de neutrons d’intensité supérieure, comme un générateur de neutron à haut flux ou un accélérateur linéaire d’électrons avec une cible de conversion appropriée. / Nuclear activities produce radioactive wastes classified following their radioactive level and decay time. An accurate characterization is necessary for efficient classification and management. Medium and high level wastes containing long lived radioactive isotopes will be stored in deep geological storage for hundreds of thousands years. At the end of this period, it is essential to ensure that the wastes do not represent any risk for humans and environment, not only from radioactive point of view, but also from stable toxic chemicals. This PhD thesis concerns the characterization of toxic chemicals and nuclear material in radioactive waste, by using neutron activation analysis, in the frame of collaboration between the Nuclear Measurement Laboratory of CEA Cadarache, France, and the Institute of Nuclear Waste Management and Reactor Safety of the research center, FZJ (Forschungszentrum Jülich GmbH), Germany. The first study is about the validation of the numerical model of the neutron activation cell MEDINA (FZJ), using MCNP Monte Carlo transport code. Simulations and measurements of prompt capture gamma rays from small samples measured in MEDINA have been compared for a number of elements of interest (beryllium, aluminum, chlorine, copper, selenium, strontium, and tantalum). The comparison was performed using different nuclear databases, resulting in satisfactory agreement and validating simulation in view of following studies. Then, the feasibility of fission delayed gamma-ray measurements of 239Pu and 235U in 225 L waste drums has been studied, considering bituminized or concrete matrixes representative of wastes produced in France and Germany. The delayed gamma emission yields were first determined from uranium and plutonium metallic samples measurements in REGAIN, the neutron activation cell of LMN, showing satisfactory consistency with published data. The useful delayed gamma signals of 239Pu and 235U, homogeneously distributed in the 225 L matrixes, were then determined by MCNP simulations using MEDINA numerical model. Weak signals of about one hundred counts per gram of 239Pu or 235U after 7200 s irradiation were obtained. Because of the high gamma emission in the bituminized waste produced in France (about 1 TBq of 137Cs per drum), the use of collimator and/or shielding is mandatory to avoid electronic saturation, making fission delayed gamma rays undetectable. However, German concrete drums being of lower activity, their corresponding active background was measured in MEDINA with a concrete mock-up, leading to detection limits between 10 and 290 g of 235U or239Pu, depending on the delayed gamma line. In order to improve these performances, the shielding of MEDINA germanium detector was optimized using MCNP calculations, resulting in gamma and neutron background reduction factors of 4 and 5, respectively. The experimental validation of the shielding efficiency was performed by implementing easy-to-build configurations in MEDINA, which confirmed the expected background reduction factors predicted by MCNP. Thanks to an optimized detector shielding, it will also be possible to use a higher neutron emission source, like a high flux neutron generator or an electron LINAC with appropriate conversion targets, in view to further reduce detection limits.