Made available in DSpace on 2014-10-09T12:55:34Z (GMT). No. of bitstreams: 0 / Made available in DSpace on 2014-10-09T14:05:54Z (GMT). No. of bitstreams: 0 / Tese (Doutoramento) / IPEN/T / Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP

Made available in DSpace on 2014-10-09T12:55:34Z (GMT). No. of bitstreams: 0 / Made available in DSpace on 2014-10-09T14:05:54Z (GMT). No. of bitstreams: 0 / As propriedades mecânicas de ferramentas confeccionadas com aços rápidos estão intimamente ligadas às características dos carbonetos dispersos na microestrutura desses materiais. Neste trabalho foi estudado o efeito do ciclo comercial de tratamento térmico de austenitização e revenimento em amostras do aço AISI/SAE M2 produzidas por metalurgia convencional, metalurgia do pó e conformação por spray. Para a realização deste estudo foram desenvolvidos métodos para a extração seletiva dos carbonetos dos tipos MC e M6C, onde M representa: vanádio, cromo, ferro, molibdênio e tungstênio, utilizando técnicas de dissolução química e eletrolítica. Estes métodos permitiram a quantificação por diferença de massa dos carbonetos do tipo M6C e MC. A extração seletiva revelou a existência de um carboneto do tipo MC com estequiometria ainda não reportada na literatura. Os parâmetros cristalográficos deste carboneto foram determinados utilizando-se o método de Rietveld. A estrutura cristalina foi refinada a partir de dados obtidos por difração de raios X, utilizando energias próximas da borda de absorção dos elementos metálicos do carboneto, através do uso de radiação de luz síncrotron. Os resultados obtidos pelo método de Rietveld permitiram determinar o grupo espacial F m -3 m para este carboneto, e que o parâmetro de rede e a estequiometria estão relacionados com a microestrutura e o teor de carbono do material antes do ciclo de tratamento térmico, porém indicando uma forte convergência para uma estequiometria comum. O conjunto dos resultados obtidos mostrou que o ciclo de tratamento térmico comercial, utilizado neste trabalho, induz ao aumento significativo da fração de carbonetos, quando comparado com o ciclo de tratamento térmico convencional descrito na literatura. A fração de carbonetos do tipo MC tem aumento mais significativo, que a do carboneto do tipo M6C, como conseqüência das alterações na estequiometria do carboneto do tipo MC. / Tese (Doutoramento) / IPEN/T / Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP

<p>Multiphase flows, such as liquid/gas and solid/gas, dominate many different areas of life, including the medical, agricultural, propulsion, and chemical industries. Gaining insight into the dynamic processes that drive these multiphase flows can therefore have far-reaching impact in many sectors of scientific research. Of key interest is the non-invasive tracking of important state properties such as the mass and temperature distributions in high optical depth multiphase flows. To accomplish this, X-ray diagnostic approaches are utilized due to their ability to probe complex phenomena without being hampered by multiple scattering that arise from complex interactions at the flow surface boundaries.</p> <p>This work accomplishes the measurement of mass distribution through time-resolved tomographic reconstructions of the liquid mass distributions in fuel sprays within liquid/gas flows. The developed diagnostic tool shown here uses a novel multiple line of sight tube source tomography setup to obtain simultaneous time-resolved two-dimensional radiographs of different spray geometries at various perspectives. Through tomographic reconstruction, these radiographs are converted into volumetric reconstructions to give a true sense of mass distribution—where exactly is the liquid mass located in the <em>x</em>, <em>y</em>, <em>z</em> spatial extents at a specific moment in time <em>t</em>? This technique is first showcased in a simple spray as a feasibility test and later applied to a more complex spray geometry and compared against other state-of- the-art diagnostics for a full quantitative understanding of the developed technique. Outside of tomography, improvements in decreasing the uncertainties in line of sight averaged mass distribution measurements in radiography imaging experiments are also showcased through source characterization efforts both for tube source and synchrotron source experiments.</p> <p>Efforts in ascertaining the temperature distributions in liquid/gas flows is done through an application of wide angle X-ray scattering, a technique that is commonly used in the materials, chemistry, and biology sciences but has yet to be widely used in the propul- sion community. These newly developed X-ray scattering measurements are accomplished through the use of a focused monochromatic beam available at the Advanced Photon Source synchrotron facility, and is applied first in calibration jets and later towards more complex dynamic sprays and multi-species liquid solutions.</p>

<p>Metalloproteins, or proteins with a metal ion cofactor, are essential for biological function of both lower and higher level organisms. These proteins provide a multitude of functions from molecular transport, such as the hemoglobin transport of oxygen, to biologically important catalytic processes. As an example case, photosystem II (PSII) is studied as a representative metalloprotein. It was chosen based on the potential impact in the energy sector due to its ability to perform water oxidation using solar based energy. Understanding mechanisms by which the Mn₄Ca cluster inside PSII, also known as the oxygen evolving complex (OEC), can store energy as redox equivalents for splitting water will be essential for future development of analogous artificial systems. By using time resolved x-ray spectroscopy, the electron structure of the metal in the protein was probed through the catalytic cycle. While the applications mentioned herein are based on PSII from spinach, the developments in time-resolved x-ray spectroscopy techniques are also applicable to other metalloproteins.</p><p></p><p>By creating a new x-ray spectrometer we were able to capture the difference in x-ray emission spectra between two compounds differing in a single metal bound ligand, i.e. Mn^IV-OH and Mn^IV=O. This both establishes the functionality of the x-ray emission spectrometer and provides useful insight into the expected changes upon an oxygen double bond formation. This change in spectroscopic signal is discussed in context of the OEC which has been hypothesized to form a Mn^IV=O state.</p><p></p><p>A new sample delivery system and further developments to the x-ray spectrometer enabled both time-resolved x-ray absorption and time-resolved x-ray emission of PSII. These experiments show the potential of synchrotron sources for time-resolved x-ray spectroscopy. From our x-ray absorption measurements we were able to follow the electronic structure changes in time using a single incident photon energy. From the kinetic traces obtained, we show possible alternative interpretations of previous results showing a delay in reduction during the final step in water oxidation. From the x-ray emission spectroscopy (XES) measurements of PSII we were able to reproduce previous results within a limited collection time and give estimates for data size requirements for metalloproteins using this spectrometer. Between the results of both these measurements, we show the improved capability for time resolved measurements at synchrotrons.</p><p>The development of x-ray free electron lasers (XFELs) has also opened many opportunities for understanding faster electronic dynamics by providing femtosecond x-ray pulse durations with ~10¹² photons per pulse. While theoretical modeling of distortions to crystallographic data have been performed, little to no work has been done to understand under what conditions such an intense pulse will have on an impact on emission spectra. Here an atomistic model was developed, and data collected, to clarify the effects of sequential ionization, i.e. two single photons absorbed by the same atom at different times during a single pulse. Experimentally we found that XFELs easily achieve flux densities that invoke a different response than is classically observed for single photon absorption and emission for Mn^II which was used as a representative case for 3d transition metals in general. We also give parameters by which the onset of this damage can be predicted and an approximation to its effect on 3d transition metals. Additionally this work guides the work of future XFEL facilities as it shows that shorter pulses, currently believed to be able to escape x-ray induced distortions to crystallography data, is not a viable method for overcoming changes in x-ray emission spectra.</p><div><br></div>

L’obtention d’un Laser à Électrons Libres X (LEL-X) compact est un objectif majeur pour le développement des lasers. Plusieurs schémas prometteurs de LEL-X ont été proposés en utilisant à la fois l’accélération d’électrons dans les plasmas et des onduleurs optiques en régime Compton ou Compton inverse. Nous avons proposé un nouveau concept de LEL-X compact baptisé Raman XFEL, en combinant la physique des LEL en régime Compton, des lasers XUV conventionnels basés sur l’interaction laser plasma, et de l’optique non-linéaire. Nous étudions dans cette thèse les étapes préalables pour déclencher un effet laser à rayons X lors de l’interaction entre un paquet d’électrons libres relativistes et un réseau optique créé par l’interférence transverse de deux impulsions laser intenses. Dans cet objectif j’ai développé un code particulaire baptisé RELIC. Les études menées avec le code RELIC nous ont permis d’étudier la dynamique d’électrons relativistes et les processus d’injection du paquet d’électrons dans le réseau optique. Grâce à RELIC, nous avons distingué de nouveaux régimes d’interaction en fonction des paramètres du paquet d’électrons, ainsi que de la géométrie du réseau optique. Ces études ont été appliquées à l’amplification du rayonnement X et appuyées par des simulations PIC. RELIC a également permis de modéliser et d’analyser la première expérience réalisée en octobre 2015 sur l’installation laser ’Salle Jaune’ au Laboratoire d’Optique Appliquée (LOA). Cette première expérience a été une étape très importante pour la validation des modèles théoriques, et pour la réalisation future d’un laser à électrons libre X Raman. / The quest for a compact X-ray laser has long been a major objective of laser science. Several schemes using optical undulators are currently considered, in order to trigger the amplification of back scattered radiation, in Compton or inverse Compton regime. We have proposed a new concept of compact XFEL based on a combination between the physics of free electron lasers, of laser-plasma interactions, and of nonlinear optics. In this thesis, we study the necessary steps to trigger a X-ray laser during the interaction between a free relativistic electron bunch and an optical lattice created by the interference of two intense transverse laser pulses. For this purpose I developed a particular tracking code dubbed RELIC. RELIC allowed us to study the dynamics and injection process of a bunch of relativistic electrons into the optical lattice. Thanks to RELIC, we distinguished several interaction regimes depending on the relativistic electron bunch parameters, and on those of the optical lattice and its geometry. These studies are applied to the X ray amplification and supported by PIC simulations. RELIC also allowed us to model and analyze the first experiment conducted in october 2015 on the ”Salle Jaune” laser facility at LOA. This first experiment was very important to validate our theoretical models, and should prove to be an essential milestone for the development of a Raman X-ray free electron laser.