Ce travail se place dans le cadre de l’utilisation des grands instruments (sources de neutrons et synchrotrons) pour l’étude de la structure et de la dynamique de matériaux désordonnés (liquides et verres). En particulier, trois études sont présentées. La première, est une étude structurale de verres Ln2O3-Al2O3-SiO2 où Ln représente les cations Sc, Y et La. Nous avons combiné des résultats obtenus par diffraction des rayons X et des neutrons et par absorption des rayons X. L’étude est focalisée sur la détermination des distances interatomiques et des coordinences pour les trois paires Si-O, Al-O et Ln-O. La seconde est une étude structurale de l’oxyde de fer FeO à l’état fondu. Des expériences de photoémission de rayons X au seuil d’absorption du fer ont été associées à des mesures de diffraction de rayons X et de neutrons. Les résultats obtenus ont permis de définir un modèle structural cohérent pour le FeO liquide. La troisième est une étude de la dynamique dans le composé CaAl2O4 fondu. La diffusion inélastique des rayons X a permis de déterminer les vitesses du son apparente et isotherme ainsi que la viscosité longitudinale. Ces mesures ont été complétées par des expériences de diffusion quasiélastique de neutrons à partir desquelles il a été possible de déterminer des coefficients de diffusion atomique. Ce travail montre l’intérêt de combiner différentes techniques expérimentales pour l’étude des verres et des milieux fondus. Il montre également la nécessité d’associer aussi des techniques de modélisation comme la dynamique moléculaire. / In this work, large scale facilities (neutron and synchrotron sources) were used for studying the structure and dynamic of disordered materials (liquids and glasses). In particular, three studies are presented. The first is a structural study of Ln2O3-Al2O3-SiO2 glasses where Ln represents the cations Sc, Y and La. We combined the results obtained from x-ray and neutron diffraction and x-ray absorption experiments. This work is focused on the determination of the interatomic distances and coordination numbers for the three pairs Si-O, Al-O and Ln-O. The second is a study of the iron oxide FeO in the liquid state. Photoemission experiments at the iron absorption edge were associated with x-ray and neutron diffraction measurements. The results obtained made it possible to define a consistent structural model for liquid FeO. The third is a study of the dynamics in CaAl2O4 melts. From inelastic x-ray scattering experiments, it was possible to determine the apparent and isothermal sound velocities as well as the longitudinal viscosity. These measurements were complemented by quasielastic neutron scattering experiments from which atomic diffusion coefficients were determined. This work shows the interest of combining various experimental techniques for studying glasses and melts and points out the need to associate also modelling techniques such as molecular dynamics simulations.

The system LiHo_<em>x</em>Y_1-<em>x</em>F₄ is a nearly perfect example of a dilute, dipolar-coupled Ising magnet and, as such, it is an ideal testing ground for many theories in statistical mechanics. At low holmium concentration (<em>x</em> = 0. 045) an unusual spin liquid or "anti-glass" state was discovered in previous work [1]. This state does not exhibit a spin glass freezing transition as is expected for a long-range interaction. Instead, it shows dynamics which are consistent with a collection of low-frequency oscillators [2]. It was also seen to have sharp features in its specific heat [3]. <br /><br /> We present heat capacity measurements on three samples at and around the concentration of the spin liquid state in zero magnetic field and in a temperature range from around 50 mK to 1 K. In contrast to previous measurements, we find no sharp features in the specific heat. The specific heat is a broad feature which is qualitatively consistent with that of a spin glass. The residual entropy as a function of <em>x</em>, obtained through a numerical integral of the data, however, is consistent with numerical simulations which predict a disappearance of spin glass ordering below a critical concentration of dipoles [4]. <br /><br /> Also presented here, is ac susceptibility data on an <em>x</em> = 0. 45 sample which exhibits a paramagnetic to ferromagnetic transition and is found to be consistent with previous work.

The system LiHo_<em>x</em>Y_1-<em>x</em>F₄ is a nearly perfect example of a dilute, dipolar-coupled Ising magnet and, as such, it is an ideal testing ground for many theories in statistical mechanics. At low holmium concentration (<em>x</em> = 0. 045) an unusual spin liquid or "anti-glass" state was discovered in previous work [1]. This state does not exhibit a spin glass freezing transition as is expected for a long-range interaction. Instead, it shows dynamics which are consistent with a collection of low-frequency oscillators [2]. It was also seen to have sharp features in its specific heat [3]. <br /><br /> We present heat capacity measurements on three samples at and around the concentration of the spin liquid state in zero magnetic field and in a temperature range from around 50 mK to 1 K. In contrast to previous measurements, we find no sharp features in the specific heat. The specific heat is a broad feature which is qualitatively consistent with that of a spin glass. The residual entropy as a function of <em>x</em>, obtained through a numerical integral of the data, however, is consistent with numerical simulations which predict a disappearance of spin glass ordering below a critical concentration of dipoles [4]. <br /><br /> Also presented here, is ac susceptibility data on an <em>x</em> = 0. 45 sample which exhibits a paramagnetic to ferromagnetic transition and is found to be consistent with previous work.

This thesis is devoted to a study of the effect of disorder on strongly correlated electrons. For non-interacting electrons, Anderson localization occurs if the amount of disorder is sufficient. For disorder-free systems, a Mott metal-insulator transition may occur if the electron-electron interactions are strong enough. The question we ask in this thesis is what happens when both disorder and interactions are present. We study the Anderson-Hubbard model, which is the simplest model to include both interactions and disorder, using a Gutzwiller variational wave function approach. We then study Anderson localization of electrons from the response of the Anderson-Hubbard Hamiltonian to an external magnetic field. An Aharonov-Bohm flux induces a persistent current in mesoscopic rings. Strong interactions result in two competing tendencies: they tend to suppress the current because of strong correlations, and they also screen the disorder potential and making the system more homogenous. We find that, for strongly interacting electrons, the localization length may be large, even though the current is suppressed by strong correlations. This unexpected result highlights how strongly correlated materials can be quiet di erent from weakly correlated ones. / Thesis (Ph.D, Physics, Engineering Physics and Astronomy) -- Queen's University, 2011-08-31 09:51:47.155

xv, 132 p. : ill. A print copy of this title is available from the UO Libraries, under the call number: SCIENCE TK7871.15.F5 H325 2007 / The effects of sulfur alloying on the electronic properties of CuIn(SeS) 2 and CuInGa(SeS) 2 materials has been investigated using sophisticated junction capacitance techniques including drive-level capacitance profiling and transient photocapacitance and photocurrent spectroscopies. CISSe and CIGSSe materials are used as absorber layers in thin-film photovoltaic devices. By characterizing the electronic properties of these materials we hope to understand how these materials can be improved to make thin-film devices with better conversion efficiencies. Sulfur widens the bandgap of these materials by moving the valence band to lower energies and the conduction band to higher energies. This significantly affects the electronic structure of these devices by increasing the activation energies of dominant acceptor levels and lowering room temperature free hole carrier densities. Using optical spectroscopies we observe a large, broad defect that also changes its apparent energetic depth with sulfur alloying. The occupation of this defect was controlled both optically and thermally, and showed a striking temperature dependence. This temperature dependence was measured by recording the relative defect signal, the ratio of the TPC signal in the defect regime to the above bandgap regime, as a function of temperature. As the temperature of the measurement was decreased, steps in the relative defect signal were observed, indicating the turning off of the thermal pathway that emptied trapped charge from the defect. Remarkably, such steps were seen at the same temperature in CISSe and CIGSSe devices with similar sulfur content. In addition, no steps were seen in CMS devices. This points to a defect state specific to the incorporation of sulfur in the absorber material. We hope that a better understanding of the electronic structure of these materials will assist in the creation of improved wide-bandgap thin-film photovoltaic devices. / Adviser: J. David Cohen

Ultrasonic wave transport in strongly scattering, disordered media is investigated via analysis of the multiply-scattered transmitted field. Measurements of transverse confinement, statistics, and correlations of the intensity were performed on an aluminum mesoglass, where aluminum beads were brazed together to form a porous slab sample. Comparison of the transverse confinement measurements with the self-consistent theory of localization was used to identify and locate a mobility edge in the sample at f = 1.1011 MHz, enabling a measurement of the critical exponent nu characterizing the Anderson transition, nu ~ 1.6–2. Infinite-range C0 correlations were observed, and observed to grow dramatically near the mobility edge, along with the C2 and C3 correlations. Measurements of the multifractal exponent Delta_2 were able to confirm the link between C0 correlations and Anderson localization. Experiments using the aluminum mesoglass with ethanol-filled pores showed evidence of two nearly-independent propagating modes, one of which appears to be characterized by a strongly renormalized diffusion coefficient. The density of states and level spacing statistics were investigated using a different mesoglass, constructed by sintering glass beads percolated on a random lattice. Direct measurements of these quantities were obtained by cutting small samples of this mesoglass, allowing individual vibrational modes to be resolved. The density of states showed a plateau extending well into the expected Debye regime, and evidence of a Boson peak was observed at low frequencies. The level spacing statistics indicated that transport in the frequency ranges measured was on the diffusive side of the mobility edge, showing agreement with the predictions of the GOE from random matrix theory. The dynamics of a suspension of bubbles were investigated using phase-based Diffusing Acoustic Wave Spectroscopy, where phase correlations were found to give additional information beyond traditional field- and intensity-based correlation measurements. / October 2015

Made available in DSpace on 2015-03-26T13:35:25Z (GMT). No. of bitstreams: 1 texto completo.pdf: 2832975 bytes, checksum: 755c3758e19c43f9d50b4a5fdc3052f6 (MD5) Previous issue date: 2007-07-20 / Fundação de Amparo a Pesquisa do Estado de Minas Gerais / The objective of this work is to verify through an experimental research of the Randorn Fuse Model, how the orientation and disorder of the fuse network influence the process of fracture of a network. To execute the experirnents a circuit of size L x L was created, with the connections among the fuses orienteded by 45° with the direction of the applied potential difference. Two types of wires were used as fuses: copper wires and steel wool wires. The experirnents consisted in applying a potential difference V in the network and to measure the current I. The results were analyzed with the objective of determining their scaling laws changing the disorder or the network size. It was concluded that even for the totally disordered networks scaling laws were not observed. It was verified that for a fixed current above a certain critical current the electric resistance of the network intreases as a power law in time and also that the rupture time of the network decreases as a logarithmic law with the current for values slightly above the critical current, while for currents much larger than the critical current the rupture time decreases as a power law. / O objetivo deste trabalho é verificar, através de um estudo experimental do Modelo Aleatório de Fusíveis, como a orientação e a desordem da rede de fusíveis influenciam o processo de fratura da rede. Para a efetivação dos experimentos foi criado um circuito de tamanho L x L, com as ligações entre os fusíveis orientadas à 45° da direção de aplicação da diferença de potencial. Foram utilizados dois tipos de fios como fusíveis: fios de cobre e fios de palha de aço. Os experimentos consistiram em aplicar uma diferença de potencial V na rede e medir a corrente I. Os resultados obtidos foram analisados com o objetivo de se determinar suas leis de escala quando a desordem ou o tamanho da rede eram variados. Concluiu-se com os resultados que mesmo para as redes totalmente desordenada não foram observadas leis de escalas. Verificou-se ainda que para uma corrente fixa acima de certa corrente crítica, a resistência elétrica da rede aumenta como uma lei de potência do tempo e também que o tempo de ruptura da rede decai como uma lei logarítmica da corrente para valores de corrente pouco acima da corrente crítica, ao passo que para valores de corrente muito acima da corrente crítica o tempo de ruptura decai como uma lei de potência.

Ces dernières décennies, l'urgence croissante de la crise énergétique et la prise de conscience qu'une grande partie de l'énergie utilisée dans le monde est dissipée sous forme de chaleur ont provoqué un engouement pour le développement de modules thermoélectriques performants. Ces dispositifs pourraient récupérer la chaleur provenant de procédés industriels ou d'autres sources, transformant un gradient de température en voltage grâce à l'effet Seebeck. Les matériaux thermoélectriques performants doivent posséder une faible conductivité thermique, une haute conductivité électrique et un grand coefficient Seebeck. L'optimisation simultanée de ces paramètres est un défi majeur pour la physique de la matière condensée et la science des matériaux. Dans l'optique d'améliorer les propriétés thermoélectriques de plusieurs matériaux prometteurs, nous explorons plusieurs stratégies dans lesquelles les défauts (substitutions atomiques, lacunes…), le désordre et le confinement dimensionnel jouent un rôle central. Nous réalisons des calculs en théorie de la fonctionnelle densité et des projections sur des orbitales de Wannier afin de construire des Hamiltoniens et des matrices dynamiques réalistes décrivant leur structure électronique et vibrationnelle dans l'espace réel. Ces paramètres sont ensuite utilisés pour calculer les propriétés de transport thermoélectrique en utilisant le formalisme de Kubo, l'équation de Boltzmann, le formalisme de Landauer et la méthode Chebyshev polynomial Green's function, qui permet un traitement exact du désordre. Nous étudions les propriétés de transport électronique et les performances thermoélectriques de deux matériaux prometteurs pour la production d'énergie à hautes températures, le titanate de strontium et l'oxyde de titane rutile. Nous obtenons un très bon accord entre nos prédictions et un grand nombre de données expérimentales. Nous montrons que l'augmentation du coefficient Seebeck observée dans les superlayers de titanate de strontium, jusque-là attribuée à des effets de confinement quantique, est en réalité très bien expliquée par l'hypothèse d'électrons délocalisés. Nous explorons les effets généraux des états résonant sur le transport électronique dans le cadre d'une étude modèle, et nous trouvons une augmentation d'un facteur six des performances thermoélectriques. Nous examinons ensuite le cas particulier du titanate de strontium, et nous montrons que les performances sont détruites par des effets de localisation si des atomes de Vanadium sont introduits comme impuretés résonantes. Nous étudions l'influence des défauts dans les matériaux bidimensionnels. Contrairement aux adatomes, nous montrons que les substitutions dans les dichalcogénures de métaux de transition ont pour effet de localiser les porteurs de charge. Nous étudions l'effet des lacunes sur le transport de phonons dans le graphène, et nous déterminons les taux de diffusion phonon-lacune. Nous obtenons un très bon accord entre notre théorie et des mesures de conductivité thermique dans des échantillons de graphène irradiés et de tailles finies / Over the past decades, the increasingly pressing need for clean energy sources and the realization that a huge proportion of the world energy consumption is wasted in heat have prompted great interest in developing efficient thermoelectric generation modules. These devices could harvest waste heat from industrial processes or other sources, turning a temperature gradient into a voltage through the Seebeck effect. Efficient thermoelectric materials should exhibit a low thermal conductivity, a high electrical conductivity and a high Seebeck coefficient. Simultaneously optimizing these parameters is a great challenge of condensed matter physics and materials science. With a view to enhance the thermoelectric properties of several promising materials, we explore several strategies in which defects (atomic substitutions, vacancies…), disorder and dimensional confinement play a crucial role. We perform density functional theory calculations and projections on Wannier orbitals to construct realistic Hamiltonians and dynamical matrices describing their electronic and vibrational structure in real space. These parameters are then used to compute the thermoelectric transport properties using the Kubo formalism, the Boltzmann transport equation, the Landauer formalism, and the Chebyshev polynomial Green's function method that allows for an exact treatment of disorder. We investigate the electronic transport properties and thermoelectric performances of two promising materials for high-temperature power generation, strontium titanate and rutile titanium dioxide. Comparison of our predictions with a wealth of experimental data yields a very good agreement. We show that the increase of the Seebeck coefficient observed in strontium titanate superlayers, until now attributed to quantum confinement effects, is in fact well explained assuming delocalized electrons. The general effects of resonant states on electronic transport are explored in a model study, showing a sixfold increase of the thermoelectric performances. The particular case of strontium titanate is then examined, and localization effects are shown to destroy the performances if Vanadium atoms are introduced as resonant impurities. The influence of defects in two-dimensional materials is investigated. Contrary to adatoms, substitutions in transition metal dichalcogenides are shown to localize the charge carriers. We study the effect of vacancies on phonon transport in graphene, and determine the phonon-vacancy scattering rate. Comparison with thermal conductivity data for irradiated and finite-size graphene samples yields a very good agreement between theory and experiments

Les contributions de cette thèse portent sur deux sujets.La première partie est dédiée à l'étude de modèles de champ moyen pour la structure électronique de matériaux avec des défauts.Dans le chapitre~ref{chap:ergodic_crystals}, nous introduisons et étudions le modèle de Hartree-Fock réduit (rHF) pour des cristaux désordonnés. Nous prouvons l'existence d'un état fondamental et établissons, pour les interactions de Yukawa (à courte portée), certaines propriétés de cet état. Dans le chapitre~ref{chap:défauts_étendus}, nous considérons des matériaux avec des défauts étendus. Dans le cas des interactions de Yukawa, nous prouvons l'existence d'un état fondamental, solution de l'équation auto-cohérente. Nous étudions également le cas de cristaux avec une faible concentration de défauts aléatoires. Dans le chapitre~ref{chap:numerical_simuation}, nous présentons des résultats de simulations numériques de systèmes aléatoires en dimension un.Dans la deuxième partie, nous étudions des modèles Monte-Carlo cinétique multi-échelles en temps. Nous prouvons, pour les trois modèles présentés au chapitre~ref{chap:kMC}, que les variables lentes convergent, dans la limite de la grande séparation des échelles de temps, vers une dynamique effective. Nos résultats sont illustrés par des simulations numériques. / The contributions of this thesis concern two topics.The first part is dedicated to the study of mean-field models for the electronic structure of materials with defects. In Chapter~ref{chap:ergodic_crystals}, we introduce and study the reduced Hartree-Fock (rHF) model for disordered crystals. We prove the existence of a ground state and establish, for (short-range)Yukawa interactions, some properties of this ground state. In Chapter~ref{chap:défauts_étendus}, we consider crystals with extended defects. Assuming Yukawa interactions, we prove the existence of an electronic ground state, solution of the self-consistent field equation. We also investigate the case of crystals with low concentration of random defects. In Chapter~ref{chap:numerical_simuation}, we present some numerical results obtained from the simulation of one-dimensional random systems.In the second part, we consider multiscale-in-time kinetic Monte Carlo models. We prove, for the three models presented in Chapter~ref{chap:kMC}, that in the limit of large time-scale separation, the slow variables converge to an effective dynamics. Our results are illustrated by numerical simulations.