This document describes work performed related to the determination of how elemental additions affect the interfacial fracture toughness of thermal barrier coatings at the bond coat/thermally grown oxide interface in gas turbines. These turbines are exposed to cyclical thermal loading, therefore a simulation was designed to model this interface in a temperature cycle between 200 K and 1000 K that included oxide growth between 2 μm and 27 μm. The fracture toughness of this interface was then determined to elucidate the function of elemental additions. It was shown that minimal concentrations of atomic species, such as hafnium and yttrium cause notable increases in the toughness of the bond coat/thermally grown oxide interface, while other species, such as sulphur, can dramatically reduce the toughness. Furthermore, it was shown that, contrary to some empirical results, the addition of platinum has a negligible effect on the fracture toughness of this interface.

This thesis deals with the idea of using accelerator driven systems for thorium transmutation into the fissile material, which can be utilized in the accelerator driven systems and in thermal nuclear reactors. Thorium occurs on Earth only in fertile isotope Th-232. It can be converted to fissile U-233 by neutron capture and subsequent beta decay. The experimental part handles the data measured by the irradiation of four thorium samples by the secondary neutrons in the QUINTA spallation target, which was irradiated with 660~MeV protons. Reaction rates for the fission and spallation products were estimated using gamma spectroscopy and activation techniques. Furthermore, Pa-233 production rates were also determined in all experimental samples. Pa-233 and fission production rates were calculated in all experimental samples using the MCNPX transport code and evaluated nuclear data for high-energy reactions. The experimental results are of a great importance for the future investigation of thorium in the accelerator driven system concept, validation of Monte-Carlo based calculation codes and validation of high-energy nuclear models.

La matiere sombre est omnipresente a plusieurs echelles de l'univers (galaxie, amas de galaxies, univers dans son ensemble). Cette matiere joue un role important en cosmologie et ne peut etre totalement expliquee par de la physique conventionnelle. Du point de vue de la physique des particules, il existe une extension du modele standard : le modele supersymetrique qui predit l'existence sous certaines conditions de nouvelles particules stables massives interagissant faiblement avec la matiere ordinaire. Outre la recherche active en detecteurs de ces nouvelles particules, il existe de nombreuses signatures indirectes accessibles aux etudes astrophysiques.<br /><br />Cette these se concentre sur une de ces signatures la desintegration de ces particules peut donner des antiprotons que nous devrions voir dans les rayons cosmiques. La presente etude s'interesse a l'evaluation du bruit de fond correspondant a ce signal i.e. les antiprotons issus de l'interactions entre ce rayonnement cosmique noyaux et la matiere du milieu interstellaire. En particulier, la meconnaissance de ce bruit de fond etant principalement due aux incertitudes liees aux parametres de diffusion, la majeure partie de cette these porte sur la propagation des noyaux.<br /><br />Le premier tiers de la these introduit la propagation des rayons cosmiques dans notre galaxie en insistant sur les processus nucleaires responsables de la fragmentation des noyaux. Dans le second tiers les differents modeles de propagation sont passes en revue et en particulier les liens entre le modele du Leaky Box et le modele de diffusion sont rappeles : la reacceleration ainsi que la convection y sont aussi discutees. Ceci donne ensuite lieu a un discussion qualitative sur l'information que nous pouvons extraire de la propagation des noyaux. Dans le dernier tiers, nous presentons finalement les solutions detaillees du modele de diffusion a deux dimensions ainsi que les contraintes obtenues sur les parametres de propagation. L'application de ces parametres au calcul du spectre de fond d'antiprotons secondaires conclut le travail de these.<br /><br />Le code de propagation realise pour les noyaux et les antiprotons sous la forme decrite dans cette these a fait ses preuves en tant qu'outil d'analyse. Son usage sera sans aucun doute d'une grande utilite pour l'experience AMS sur la station spatiale internationale en 2003.

L'objectif de ce travail de thèse est d'examiner le rôle de la sous-criticité du coeur, en tant que moyen pour améliorer la sûreté des systèmes nucléaires innovants, notamment des réacteurs à sel fondu, dédiés à la production d'énergie et/ou à la transmutation/incinération des déchets nucléaires. La sûreté intrinsèque est considérée comme l'objectif ultime de cette amélioration. Une tentative d'appliquer une approche systématisée pour l'analyse de la contribution de la sous-criticitité au comportement intrinsèque des systèmes hybrides est effectuée. Les résultats de cette étude prouvent que la sous-criticité améliore bien la sûreté des réacteurs nucléaires, et même, dans certaines configurations, permet d'attendre la sûreté intrinsèque. Dans tous les cas, un choix approprié du niveau de sous-criticité rend les transitoires plus lents et monotones. Il est montré que le point faible pour des systèmes hybrides avec une source indépendante de neutrons sont les transitoires thermo-hydrauliques non protégés tandis que pour des hybrides avec des sources couplées ce sont les transitoires de réactivité. Pour surmonter les inconvénients intrinsèques à ces deux types de systèmes hybrides, un nouveau principe de réalisation des systèmes hybrides couplés est proposé (concept DENNY). De plus, des approches, qui permettent de remédier à certains problèmes de sûreté, sont proposées. Une analyse préliminaire du potentiel de sûreté intrinsèque pour un réacteur à sel fondu avec spectre rapide (concept REBUS) est effectuée. Enfin, le potentiel des sources alternatives de neutrons basées sur des réactions thermonucléaires et photo-nucléaires est examiné.

L'objectif principal de l'expérience Borexino est "la détection en temps réel" des neutrinos solaires de la raie du béryllium à 862keV. Outre cette mesure pionnière dans le domaine des neutrinos de basse énergie, Borexino pourra mesurer les neutrinos solaires au-dessus du MeV (neutrinos du 8B et neutrinos pep), les neutrinos de réacteurs nucléaires (d'énergie moyenne d'environ 3 MeV) et les neutrinos de supernovae (dont le spectre en énergie s'étend jusqu'à quelques dizaines de MeV). Le présent travail est consacré principalement à l'étude des neutrinos de réacteurs nucléaires. Ce domaine a été récemment enrichi par les résultats de KamLAND, qui ont grandement amélioré la détermination des paramètres d'oscillations des neutrinos. Dans l'objectif de mesurer ces événements au dessus du MeV, la collaboration Borexino a confié au groupe du PCC, Collège de France, le développement d'un système de numérisation rapide fonctionnant à 400 MHz: les cartes FADC. Elles ont été conçues au laboratoire et nous les avons finalisées au début de l'année 2002. Les premières cartes implantées dans l'électronique d'acquisition de Borexino nous ont permis de contrôler leurs fonctionnements et celui du programme d'acquisition. Elles ont été également installées sur le prototype de Borexino, CTF. Les données correspondantes sont analysées en vue de mettre une limite sur le bruit de fond attendu dans Borexino pour la mesure des neutrinos de réacteurs nucléaires.

Ce mémoire de HDR traite d'une dizaine d'années de travaux autour de la modélisation des réactions de spallation. Ces réactions sont définies comme l'interaction nucléaire entre une particule légère, le plus souvent un nucléon, et un noyau atomique à une énergie de l'ordre de 100 MeV à 2-3 GeV. Deux étapes les caractérisent. Une phase rapide, la réaction directe appelée aussi cascade intra- nucléaire, et une phase plus lente, la désexcitation du noyau issu de la première phase. À partir de l'association du code développé par le groupe pour la cascade, INCL4, et du code de désexcitation Abla, de GSI, sont présentés les différentes facettes des réactions de spallation. D'abord la physique et les codes sont présentés, ce sont ensuite les différents types de validations des modèles qui sont exposés, puis les multiples domaines dans lesquels la modélisation de la spallation joue un rôle, pour enfin, tirant profit de tout ce qui aura été dit et d'autres travaux passés, montrer les différents voies qu'il reste à explorer ou redécouvrir.

No description available.

Neste trabalho apresentamos um estudo das reações de spallation a energias interme- diárias em núcleos actinídeos e pré-actinídeos. Para esta finalidade foi utilizado o modelo de Monte Carlo CRISP (Colaboração Rio-São Paulo), que neste estudo foi importante na reprodução da distribuição de massa de produtos residuais e as seções de choque de fissão e espalação. Estes observáveis são importantes para o estudo de Reatores Hibridos ADS considerado como dispositivos promissores para a transmutação de resíduos nucle- ares. Os modelos físicos necessários para uma correta simulação de dados experimentais foram já implementadas no CRISP, como o modelo de evaporação para emissão de par- tículas descrito por Weisskopf de 1937, e para fissão o clássico modelo de Bohr/Wheeler de 1939. Para a obtenção da distribuição dos fragmentos de massa de fissão o CRISP conta também com um modelo baseado na parametrização multimodal de fissão, que si- mula os processos de fissão simétrica e assimétrica predominantes em altas e baixas ener- gias, respectivamente. Os resultados obtidos do CRISP depois da aplicação dos modelos mencionados, foram os rendimentos de massa dos fragmentos residuais, os quais foram analisadas para o cálculo da seção de choque de fissão e espalação mediante uma fórmula implementada no modelo. Com o resultado se fez o gráfico da distribuição de massa para cada uma das reações analisadas. Uma das reações estudadas foi a reação induzida por fótons de Bremsstrahlung com energias máximas de 50 e 3500 MeV em um alvo de 181 Ta, calculando a distribuição de massa de fissão e espalação, mostrando bons resultados de acordo com os dados experimentais. Nas reações induzidas por prótons foram calcula- das as seções de choque de fissão e espalação assim como sua respectiva distribuição de massa dos produtos residuais. Neste caso estudamos duas reações, sendo: a reação p (1 GeV) + 208 Pb, e a reação de p (660 MeV) + 238 U. Para a primeira reação com chumbo os resultados do CRISP foram comparados com dados experimentais, e também com os resultados obtidos do modelo MCNPX-Bertini do trabalho de Baylac-Domengetroy de 2003, que simulou a mesma reação com chumbo. Obtendo-se melhores resultados com o CRISP mas com uma superestimação de dados no final da distribuição calculada. No caso do urânio, foi necessário usar a chamada fissão superassimétrica porque a distribuição de massa experimental é mais complexa e o modelo multimodal clássico não é suficiente para sua correta simulação. Foi também estudado as reações induzidas por dêuterons usando o modelo CRISP, mostrando os resultados da distribuição de massa para 197 Au e 208 Pb com algumas limitações do modelo para este tipo de reações. / In this work we present a study of the spallation reactions by intermediate energies in actinide and pre-actinide nuclei. For this purpose we used the Monte Carlo model CRISP (Rio-São Paulo Collaboration), for our study was important in the reproduction of the mass distribution of waste products and the total fission and spallation cross secti- ons. These observables are important for the study of Accelerator Driven System Reac- tors (ADS) considered as promising devices for the transmutation of nuclear waste. The physical models needed for a correct simulation of experimental data were already imple- mented in CRISP, such as the evaporation model for emission of particles described by Weisskopf in 1937, and the classical Bohr/Wheeler model in 1939, for fission. To obtain the fragment mass distribution for fission, CRISP has a model based on multimodal fis- sion parameter, which simulates the processes called symmetric and asymmetric fission that are predominant at high and low energies respectively. The CRISP results, obtai- ned after the application of the above mentioned models, were the mass yield of residual fragments, which were analyzed to calculate the fission and spallation cross section using a formula that was implemented in the CRISP model. With these result was obtained the mass distribution for each reaction analyzed. One of the reactions studied was a re- action induced by Bremsstrahlung photons with endpoint energies of 50 MeV and 3500 in a target 181 Ta, calculating the fission and spallation mass distribution, showing good results according the experimental data. In the reactions induced by protons were cal- culated fission and spallation cross sections as well as their respective mass distribution of the residual products. In this case we study two reactions, as follows: p (1 GeV) + 208 , and p (660 MeV) + 238 U. For the first reaction with lead, the results of CRISP were compared with experimental data and with results obtained of MCNPX-Bertini model of Baylac-Domengetroy work in 2003, simulated the same reaction with lead. Obtaining better results with CRISP, but with data-overestimated at the end of calculated distribu- tion. For uranium it was necessary to use the called superasymmetric fission, because the experimental mass distribution is more complicated and the classical model is not suffi- cient for a correct simulation. Has been also studied the reactions induced by deuterons using the CRISP model, showing the mass distribution

Neste trabalho apresentamos um estudo das reações de spallation a energias interme- diárias em núcleos actinídeos e pré-actinídeos. Para esta finalidade foi utilizado o modelo de Monte Carlo CRISP (Colaboração Rio-São Paulo), que neste estudo foi importante na reprodução da distribuição de massa de produtos residuais e as seções de choque de fissão e espalação. Estes observáveis são importantes para o estudo de Reatores Hibridos ADS considerado como dispositivos promissores para a transmutação de resíduos nucle- ares. Os modelos físicos necessários para uma correta simulação de dados experimentais foram já implementadas no CRISP, como o modelo de evaporação para emissão de par- tículas descrito por Weisskopf de 1937, e para fissão o clássico modelo de Bohr/Wheeler de 1939. Para a obtenção da distribuição dos fragmentos de massa de fissão o CRISP conta também com um modelo baseado na parametrização multimodal de fissão, que si- mula os processos de fissão simétrica e assimétrica predominantes em altas e baixas ener- gias, respectivamente. Os resultados obtidos do CRISP depois da aplicação dos modelos mencionados, foram os rendimentos de massa dos fragmentos residuais, os quais foram analisadas para o cálculo da seção de choque de fissão e espalação mediante uma fórmula implementada no modelo. Com o resultado se fez o gráfico da distribuição de massa para cada uma das reações analisadas. Uma das reações estudadas foi a reação induzida por fótons de Bremsstrahlung com energias máximas de 50 e 3500 MeV em um alvo de 181 Ta, calculando a distribuição de massa de fissão e espalação, mostrando bons resultados de acordo com os dados experimentais. Nas reações induzidas por prótons foram calcula- das as seções de choque de fissão e espalação assim como sua respectiva distribuição de massa dos produtos residuais. Neste caso estudamos duas reações, sendo: a reação p (1 GeV) + 208 Pb, e a reação de p (660 MeV) + 238 U. Para a primeira reação com chumbo os resultados do CRISP foram comparados com dados experimentais, e também com os resultados obtidos do modelo MCNPX-Bertini do trabalho de Baylac-Domengetroy de 2003, que simulou a mesma reação com chumbo. Obtendo-se melhores resultados com o CRISP mas com uma superestimação de dados no final da distribuição calculada. No caso do urânio, foi necessário usar a chamada fissão superassimétrica porque a distribuição de massa experimental é mais complexa e o modelo multimodal clássico não é suficiente para sua correta simulação. Foi também estudado as reações induzidas por dêuterons usando o modelo CRISP, mostrando os resultados da distribuição de massa para 197 Au e 208 Pb com algumas limitações do modelo para este tipo de reações. / In this work we present a study of the spallation reactions by intermediate energies in actinide and pre-actinide nuclei. For this purpose we used the Monte Carlo model CRISP (Rio-São Paulo Collaboration), for our study was important in the reproduction of the mass distribution of waste products and the total fission and spallation cross secti- ons. These observables are important for the study of Accelerator Driven System Reac- tors (ADS) considered as promising devices for the transmutation of nuclear waste. The physical models needed for a correct simulation of experimental data were already imple- mented in CRISP, such as the evaporation model for emission of particles described by Weisskopf in 1937, and the classical Bohr/Wheeler model in 1939, for fission. To obtain the fragment mass distribution for fission, CRISP has a model based on multimodal fis- sion parameter, which simulates the processes called symmetric and asymmetric fission that are predominant at high and low energies respectively. The CRISP results, obtai- ned after the application of the above mentioned models, were the mass yield of residual fragments, which were analyzed to calculate the fission and spallation cross section using a formula that was implemented in the CRISP model. With these result was obtained the mass distribution for each reaction analyzed. One of the reactions studied was a re- action induced by Bremsstrahlung photons with endpoint energies of 50 MeV and 3500 in a target 181 Ta, calculating the fission and spallation mass distribution, showing good results according the experimental data. In the reactions induced by protons were cal- culated fission and spallation cross sections as well as their respective mass distribution of the residual products. In this case we study two reactions, as follows: p (1 GeV) + 208 , and p (660 MeV) + 238 U. For the first reaction with lead, the results of CRISP were compared with experimental data and with results obtained of MCNPX-Bertini model of Baylac-Domengetroy work in 2003, simulated the same reaction with lead. Obtaining better results with CRISP, but with data-overestimated at the end of calculated distribu- tion. For uranium it was necessary to use the called superasymmetric fission, because the experimental mass distribution is more complicated and the classical model is not suffi- cient for a correct simulation. Has been also studied the reactions induced by deuterons using the CRISP model, showing the mass distribution

The most promising applications for targeted alpha-therapy with astatine-211 (At-211) include treatments of disseminated microscopic disease, the major medical problem for cancer treatment. The primary advantages of targeted alpha-therapy with At-211 are that the alpha-particle radiation is densely ionizing, translating to high relative biological effectiveness (RBE), and short-range, minimizing damage to surrounding healthy tissues. In addition, theranostic imaging with I-123 surrogates has shown promise for developing new therapies with At-211 and translating them to the clinic. Currently, Canada does not have a way of producing At-211 by conventional methods because it lacks alpha-particle accelerators with necessary beam energy and intensity. The work presented here was aimed at studying the Rn-211/At-211 generator system as an alternative production strategy by leveraging TRIUMF's ability to produce rare isotopes. Recognizing that TRIUMF provided production opportunities for a variety of astatine isotopes, this work also originally hypothesized and evaluated the use of At-209 as a novel isotope for preclinical Single Photon Emission Computed Tomography (SPECT) with applications to At-211 therapy research. At TRIUMF's Isotope Separator and Accelerator (ISAC) facility, mass separated ion beams of short­-lived francium isotopes were implanted into NaCl targets where Rn-211 or At-209 were produced by radioactive decay, in situ. This effort required methodological developments for safely relocating the implanted radioactivity to the radiochemistry laboratory for recovery in solution. For multiple production runs, Rn-211 was quantitatively transferred from solid NaCl to solution (dodecane) from which At-211 was efficiently extracted and evaluated for clinical applicability. This validated the use of dodecane for capturing Rn-211 as an elegant approach to storing and shipping Rn-211/At-211 in the future. Po-207 contamination (also produced by Rn-211 decay) was removed using a granular tellurium (Te) column before proceeding with biomolecule labelling. Although the produced quantities were small, the pure At-211 samples demonstrated these efforts to have a clear path of translation to animal studies. For the first time in history, SPECT/CT was evaluated for measuring At-209 radioactivity distributions using high energy collimation. The spectrum detected for At-209 by the SPECT camera presented several photopeaks (energy windows) for reconstruction. The 77-90 Po X­-ray photopeak reconstructions were found to provide the best images overall, in terms of resolution/contrast and uniformity. Collectively, these experiments helped establish guidelines for determining the optimal injected radioactivity, depending on scan parameters. Moreover, At-209-based SPECT demonstrated potential for pursuing image-­based dosimetry in mouse tumour models, in the future. Simultaneous SPECT imaging with At-209 and I-123 was demonstrated to be feasible, supporting the future evaluation of At-209 for studying/validating I-123 surrogates for clinical image-based At-211 dosimetry. This work also pursued a novel strategy for labelling cancer targeting peptides with At-211, using octreotate (TATE, a somatostatin analogue for targeting tumour cells, mostly neuroendocrine tumours) prepared with or without N-terminus PEGylation (PEG2), followed by conjugation with a closo-decaborate linking moiety (B10) for attaching At-211. Binding affinity and in vivo biodistributions for the modified peptides were determined using iodine surrogates. The results indicated that B10-PEG2-TATE retained target binding affinity but that the labelling reaction with iodine degraded this binding affinity significantly, and although having high in vivo stability, no I-123-B10-PEG2-TATE tumour uptake was observed by SPECT in a mouse tumour model positive for the somatostatin receptor (sstr2a). This suggested that further improvements are required for labelling. A new method for producing At-211 at TRIUMF is established, and At-209-­based SPECT imaging is now demonstrated as a new preclinical technology to measure astatine biodistributions in vivo for developing new radiopharmaceuticals with At-211. Combined with the theranostic peptide labelling efforts with iodine, these efforts provide a foundation for future endeavours with At-211-­based alpha-therapy at TRIUMF. All procedures were performed safely and rapidly, suitable for preclinical evaluations. All animal studies received institutional ethics approval from the University of British Columbia (UBC). / Graduate