O fator de Dancoff, em sua formulação clássica, corrige a corrente de nêutrons incidente na superfície de uma vareta combustível devido à presença das demais varetas da célula. Alternativamente, esse fator pode ser interpretado como a probabilidade de um nêutron oriundo de uma vareta de combustível entrar em outra vareta sem colidir no moderador ou no revestimento. Para combustíveis perfeitamente absorvedores essas definições são equivalentes. Entretanto, quando se assume a hipótese de absorção parcial no combustível, essa equivalência não se verifica. Então, os fatores de Dancoff devem ser determinados em termos de probabilidades de colisão. Ao longo dos últimos anos, vários trabalhos, usando ambas as definições, vêm relatando melhorias no cálculo dos fatores Dancoff. Neste trabalho, esses fatores são determinados através do método de probabilidades de colisão para células em geometria cluster com contorno externo quadrado, assumindo-se absorção total (Black Dancoff Factors) e parcial (Grey Dancoff Factors) no combustível. A validação dos resultados é feita através de comparações com a célula cilíndrica equivalente. O cálculo é realizado considerando-se reflexão especular, para a célula quadrada, e condição de contorno difusa (white) para a célula cilíndrica equivalente. Os resultados obtidos, com o aumento do tamanho das células, evidenciam o comportamento assintótico da solução. Além disso, são computados fatores de Dancoff para as células canadenses CANDU-37 e CANFLEX por ambas as metodologias de cálculo, direta e probabilística. Finalmente, os fatores de multiplicação efetivo, keff, para as células com contorno externo quadrado e a cilíndrica equivalente, são determinados e as diferenças registradas para os casos onde se assumem as hipóteses de absorção total e parcial. / In its classical formulation, the Dancoff factor for a perfectly absorbing fuel rod is defined as the relative reduction in the incurrent of resonance neutrons into the rod in the presence of neighboring rods, as compared to the incurrent into a single fuel rod immersed in an infinite moderator. Alternatively, this factor can be viewed as the probability that a neutron emerging from the surface of a fuel rod will enter another fuel rod without any collision in the moderator or cladding. For perfectly absorbing fuel these definitions are equivalent. In the last years, several works appeared in literature reporting improvements in the calculation of Dancoff factors, using both the classical and the collision probability definitions. In this work, we step further reporting Dancoff factors for perfectly absorbing (Black) and partially absorbing (Grey) fuel rods calculated by the collision probability method, in cluster cells with square outer boundaries. In order to validate the results, comparisons are made with the equivalent cylindricalized cell in hypothetical test cases. The calculation is performed considering specularly reflecting boundary conditions, for the square lattice, and diffusive reflecting boundary conditions, for the cylindrical geometry. The results show the expected asymptotic behavior of the solution with increasing cell sizes. In addition, Dancoff factors are computed for the Canadian cells CANDU-37 and CANFLEX by the Monte Carlo and Direct methods. Finally, the effective multiplication factors, keff, for these cells (cluster cell with square outer boundaries and the equivalent cylindricalized cell) are also computed, and the differences reported for the cases using the perfect and partial absorption assumptions.

O fator de Dancoff, em sua formulação clássica, corrige a corrente de nêutrons incidente na superfície de uma vareta combustível devido à presença das demais varetas da célula. Alternativamente, esse fator pode ser interpretado como a probabilidade de um nêutron oriundo de uma vareta de combustível entrar em outra vareta sem colidir no moderador ou no revestimento. Para combustíveis perfeitamente absorvedores essas definições são equivalentes. Entretanto, quando se assume a hipótese de absorção parcial no combustível, essa equivalência não se verifica. Então, os fatores de Dancoff devem ser determinados em termos de probabilidades de colisão. Ao longo dos últimos anos, vários trabalhos, usando ambas as definições, vêm relatando melhorias no cálculo dos fatores Dancoff. Neste trabalho, esses fatores são determinados através do método de probabilidades de colisão para células em geometria cluster com contorno externo quadrado, assumindo-se absorção total (Black Dancoff Factors) e parcial (Grey Dancoff Factors) no combustível. A validação dos resultados é feita através de comparações com a célula cilíndrica equivalente. O cálculo é realizado considerando-se reflexão especular, para a célula quadrada, e condição de contorno difusa (white) para a célula cilíndrica equivalente. Os resultados obtidos, com o aumento do tamanho das células, evidenciam o comportamento assintótico da solução. Além disso, são computados fatores de Dancoff para as células canadenses CANDU-37 e CANFLEX por ambas as metodologias de cálculo, direta e probabilística. Finalmente, os fatores de multiplicação efetivo, keff, para as células com contorno externo quadrado e a cilíndrica equivalente, são determinados e as diferenças registradas para os casos onde se assumem as hipóteses de absorção total e parcial. / In its classical formulation, the Dancoff factor for a perfectly absorbing fuel rod is defined as the relative reduction in the incurrent of resonance neutrons into the rod in the presence of neighboring rods, as compared to the incurrent into a single fuel rod immersed in an infinite moderator. Alternatively, this factor can be viewed as the probability that a neutron emerging from the surface of a fuel rod will enter another fuel rod without any collision in the moderator or cladding. For perfectly absorbing fuel these definitions are equivalent. In the last years, several works appeared in literature reporting improvements in the calculation of Dancoff factors, using both the classical and the collision probability definitions. In this work, we step further reporting Dancoff factors for perfectly absorbing (Black) and partially absorbing (Grey) fuel rods calculated by the collision probability method, in cluster cells with square outer boundaries. In order to validate the results, comparisons are made with the equivalent cylindricalized cell in hypothetical test cases. The calculation is performed considering specularly reflecting boundary conditions, for the square lattice, and diffusive reflecting boundary conditions, for the cylindrical geometry. The results show the expected asymptotic behavior of the solution with increasing cell sizes. In addition, Dancoff factors are computed for the Canadian cells CANDU-37 and CANFLEX by the Monte Carlo and Direct methods. Finally, the effective multiplication factors, keff, for these cells (cluster cell with square outer boundaries and the equivalent cylindricalized cell) are also computed, and the differences reported for the cases using the perfect and partial absorption assumptions.

O fator de Dancoff, em sua formulação clássica, corrige a corrente de nêutrons incidente na superfície de uma vareta combustível devido à presença das demais varetas da célula. Alternativamente, esse fator pode ser interpretado como a probabilidade de um nêutron oriundo de uma vareta de combustível entrar em outra vareta sem colidir no moderador ou no revestimento. Para combustíveis perfeitamente absorvedores essas definições são equivalentes. Entretanto, quando se assume a hipótese de absorção parcial no combustível, essa equivalência não se verifica. Então, os fatores de Dancoff devem ser determinados em termos de probabilidades de colisão. Ao longo dos últimos anos, vários trabalhos, usando ambas as definições, vêm relatando melhorias no cálculo dos fatores Dancoff. Neste trabalho, esses fatores são determinados através do método de probabilidades de colisão para células em geometria cluster com contorno externo quadrado, assumindo-se absorção total (Black Dancoff Factors) e parcial (Grey Dancoff Factors) no combustível. A validação dos resultados é feita através de comparações com a célula cilíndrica equivalente. O cálculo é realizado considerando-se reflexão especular, para a célula quadrada, e condição de contorno difusa (white) para a célula cilíndrica equivalente. Os resultados obtidos, com o aumento do tamanho das células, evidenciam o comportamento assintótico da solução. Além disso, são computados fatores de Dancoff para as células canadenses CANDU-37 e CANFLEX por ambas as metodologias de cálculo, direta e probabilística. Finalmente, os fatores de multiplicação efetivo, keff, para as células com contorno externo quadrado e a cilíndrica equivalente, são determinados e as diferenças registradas para os casos onde se assumem as hipóteses de absorção total e parcial. / In its classical formulation, the Dancoff factor for a perfectly absorbing fuel rod is defined as the relative reduction in the incurrent of resonance neutrons into the rod in the presence of neighboring rods, as compared to the incurrent into a single fuel rod immersed in an infinite moderator. Alternatively, this factor can be viewed as the probability that a neutron emerging from the surface of a fuel rod will enter another fuel rod without any collision in the moderator or cladding. For perfectly absorbing fuel these definitions are equivalent. In the last years, several works appeared in literature reporting improvements in the calculation of Dancoff factors, using both the classical and the collision probability definitions. In this work, we step further reporting Dancoff factors for perfectly absorbing (Black) and partially absorbing (Grey) fuel rods calculated by the collision probability method, in cluster cells with square outer boundaries. In order to validate the results, comparisons are made with the equivalent cylindricalized cell in hypothetical test cases. The calculation is performed considering specularly reflecting boundary conditions, for the square lattice, and diffusive reflecting boundary conditions, for the cylindrical geometry. The results show the expected asymptotic behavior of the solution with increasing cell sizes. In addition, Dancoff factors are computed for the Canadian cells CANDU-37 and CANFLEX by the Monte Carlo and Direct methods. Finally, the effective multiplication factors, keff, for these cells (cluster cell with square outer boundaries and the equivalent cylindricalized cell) are also computed, and the differences reported for the cases using the perfect and partial absorption assumptions.

<p>Clusters are finite ensembles of atoms or molecules with sizes in the nanometer regime (<i>i.e.</i> nanoparticles). This thesis present results on the geometric and electronic structure of homogeneous and heterogeneous combinations of atoms and molecules. The systems have been studied with synchrotron radiation and valence, core and Auger electron spectroscopic techniques.</p><p>The first theme of the thesis is that of mixed clusters. It is shown that by varying the cluster production technique both structures that are close to that predicted by equilibrium considerations can be attained as well as far from equilibrium structures.</p><p>Electronic processes following ionization constitute the second theme. The post-collision interaction phenomenon, energy exchange between the photo- and the Auger electrons, is shown to be different in clusters of argon, krypton and xenon. A model is proposed that takes polarization screening in the final state into account. This result is of general character and should be applicable to the analysis of core level photoelectron and Auger electron spectra of insulating and semi-conducting bulk materials as well.</p><p>Interatomic Coloumbic Decay is a process that can occur in the condensed phases of weakly bonded systems. Results on the time-scale of the process in Ne clusters and mixed Ar/Ne clusters are herein discussed, as well observations of resonant contributions to the process. In analogy to Auger <i>vis-à-vis</i> Resonant Auger it is found that to the ICD process there is a corresponding Resonant ICD process possible. This has later been observed in other systems and by theoretical calculations as well in subsequent works by other groups.</p><p>Delocalization of dicationic valence final states in the hydrogen bonded ammonia clusters and aqueous ammonia has also been investigated by Auger electron spectroscopy. With those results it was possible to assign a previously observed feature in the Auger electron spectrum of solid ammonia.</p>

Clusters are finite ensembles of atoms or molecules with sizes in the nanometer regime (i.e. nanoparticles). This thesis present results on the geometric and electronic structure of homogeneous and heterogeneous combinations of atoms and molecules. The systems have been studied with synchrotron radiation and valence, core and Auger electron spectroscopic techniques. The first theme of the thesis is that of mixed clusters. It is shown that by varying the cluster production technique both structures that are close to that predicted by equilibrium considerations can be attained as well as far from equilibrium structures. Electronic processes following ionization constitute the second theme. The post-collision interaction phenomenon, energy exchange between the photo- and the Auger electrons, is shown to be different in clusters of argon, krypton and xenon. A model is proposed that takes polarization screening in the final state into account. This result is of general character and should be applicable to the analysis of core level photoelectron and Auger electron spectra of insulating and semi-conducting bulk materials as well. Interatomic Coloumbic Decay is a process that can occur in the condensed phases of weakly bonded systems. Results on the time-scale of the process in Ne clusters and mixed Ar/Ne clusters are herein discussed, as well observations of resonant contributions to the process. In analogy to Auger vis-à-vis Resonant Auger it is found that to the ICD process there is a corresponding Resonant ICD process possible. This has later been observed in other systems and by theoretical calculations as well in subsequent works by other groups. Delocalization of dicationic valence final states in the hydrogen bonded ammonia clusters and aqueous ammonia has also been investigated by Auger electron spectroscopy. With those results it was possible to assign a previously observed feature in the Auger electron spectrum of solid ammonia.