Strong correlations caused by interaction in systems of electrons can bring about unusual physical phenomena due to many-body quantum effects that cannot properly be captured by standard electronic structure methods like density functional theory. In this thesis, we apply the state-of-the-art continuous-time quantum Monte Carlo algorithm in hybridization expansion (CT-HYB) for the strongly correlated multi-orbital Anderson impurity model (AIM) to the solution of models of magnetic impurities on metallic surfaces and, via dynamical mean-field theory (DMFT), to the solution of a lattice model, the multi-orbital Hubbard model with Hund's coupling. A concise introduction to the theoretical background focuses on information directly relevant to the understanding of applied models, methods, and the interpretation of results. It starts with a discussion of the AIM with its parameters and its solution in the path integral formalism, the basis of the CT-HYB algorithm. We consider its derivation and implementation in some detail before reviewing the DMFT approach to correlated lattice models and the interpretation of the single-particle Green's function. We review two algorithmic developments for the CT-HYB algorithm that help to increase the performance of calculations especially in case of a complex structure of the interaction matrix and allow the precise calculation of self-energies and vertex functions also at intermediate and higher frequencies. Our comparative analysis of Kondo screening in the cobalt on copper impurity system points out the importance of an accurate interaction matrix for qualitatively correct Kondo temperatures and the relevance of all d-orbitals in that case. Theoretical modeling of cobalt impurities in copper "atomic wires" fails to reproduce variations and partial absence of Kondo resonances depending on the wire size. We analyze the dependence of results on parameters and consider possible reasons for the discrepancy. Different Kondo temperatures of iron adatoms adsorbed on clean or oxygen-reconstructed niobium in the normal state are qualitatively reproduced, with the adsorption distance identified as major factor and implications for the superconducting state pointed out. Moving on to lattice problems, we demonstrate the connection between Hund's coupling, shown to cause first-order character of the interaction-driven Mott transition at half-filling in the two-orbital Hubbard model, and a phase separation zone ending in a quantum critical point at finite doping. We touch on similarities in realistic models of iron-pnictide superconductors. We analyze the manifestation of the compressibility divergence at the finite-temperature critical points away from half-filling in the eigenbasis of the two-particle generalized susceptibility. A threshold for impurity susceptibility eigenvalues that indicates divergence of the DMFT lattice compressibility and distinguishes thermodynamic stability and instability of DMFT solutions is determined. / Wechselwirkungsbedingt stark korrelierte Elektronensysteme können wegen Mehrteilcheneffekten ungewöhnliche Physik aufweisen, die Standardmethoden für elektronische Struktur wie die Dichtefunktionaltheorie nicht erfassen. Diese Dissertation handelt von der Anwendung des Quanten-Monte Carlo Algorithmus in kontinuierlicher Zeit mit Reihenentwicklung in der Hybridisierung (CT-HYB), aktuellster Stand der Technik für das stark korrelierte Anderson-Modell für Störstellen (AIM), auf magnetische Adatome auf Metalloberflächen und, im Rahmen der dynamischen Molekularfeldtheorie (DMFT), auf das Mehrorbital-Hubbard-Modell mit Hundscher Kopplung. Eine kurze Einführung fokussiert den für das Verständnis der Modelle, Methoden, und Interpretationen relevanten theoretischen Hintergrund. Sie beginnt mit dem AIM, seinen Parametern, und seiner Lösung im Pfadintegralformalismus, welche Grundlage des CT-HYB Algorithmus ist. Wir betrachten dessen Herleitung und Implementation im Detail, bevor wir einen Überblick über den DMFT-Zugang zu korrelierten Gittermodellen und die Interpretation der Einteilchen-Greenschen Funktion geben. Wir berichten von zwei algorithmischen Entwicklungen für CT-HYB, die helfen, die Geschwindigkeit der Rechnungen besonders in Fällen einer lokalen Wechselwirkung komplexer Form zu erhöhen und die präzise Berechnung von Selbstenergien und Vertexfunktionen auch bei mittleren und höheren Frequenzen erlauben. Unsere Analyse der Kondo-Abschirmung in Kobalt-Adatomen auf Kupfer weist auf die Bedeutung einer akkuraten Wechselwirkungsmatrix für korrekte Kondo-Temperaturen und die Relevanz aller d-Orbitale hin. Die Variation der Kondo-Resonanz von Kobalt in "atomaren Drähten" aus Kupfer mit der Anzahl der Atome kann unsere theoretische Modellierung nicht nachvollziehen. Wir untersuchen die Abhängigkeit der Ergebnisse von Parametern und diskutieren mögliche Ursachen. Kondo-Temperaturen von Eisen-Adatomen auf sauberer oder Sauerstoff-rekonstruierter Niob-Oberfläche werden im Normalzustand qualitativ reproduziert, der Adsorptionsabstand als wichtiger Faktor identifiziert, und auf die Folgen für den supraleitenden Zustand hingewiesen. Wir wenden uns dem Hubbard-Modell eines Gitters mit zwei Orbitalen pro Platz zu und zeigen den Zusammenhang zwischen Hundscher Kopplung, Ursache der Diskontinuität des Mott-Übergangs bei halber Füllung, und einer Phasenseparationszone endend in einem quantenkritischen Punkt bei endlicher Dotierung. Wir reißen Parallelen in realistischeren Eisenpniktid-Modellen an. Zuletzt sehen wir, wie sich die Kompressibilitätsdivergenz an den kritischen Punkten bei endlicher Temperatur abseits halber Füllung in den Eigenwerten der verallgemeinerten lokalen Suszeptibilität ausprägt und bestimmen für sie eine Schwelle, an der die DMFT-Gitterkompressibilität divergiert und deren Unterschreitung eine thermodynamisch instabile DMFT-Lösung anzeigt.

El objetivo de esta tesis es la síntesis de películas delgadas de SnS utilizando técnicas de bajo coste con el fin de fabricar células solares. Nuestra contribución radica en estudiar nuevos materiales susceptibles de ser utilizados para aplicaciones fotovoltaicas, y que puedan ser preparados con técnicas de bajo coste como la técnica de Pyrolysis de Spray Químico (CSP) y caracterizar algunos materiales elegidos para este fin como el Sulfuro de Estaño (SnS). Se han fabricado células solares a partir de la disposición de capas: Mo / SnS / Tampón / i-ZnO / ZnO: Al / Al / Metal. Las capas de buffer serían: In2S3 o CdS. En la primera etapa hemos procedido a la optimización de los parámetros de deposición de películas delgadas de SnS usando la técnica de la CSP, -Variación de la relación [S] / [Sn]. -Variación de la temperatura del substrato. -Variación de la naturaleza del sustrato utilizando sustrato como vidrio, óxido de estaño de indio (ITO) y vidrio recubierto de molibdeno. Las fuentes de productos químicos y disolventes utilizados son: - Cloruro de dihidrato dihidratado para Tin (Sn), Thiourea, Agua destilada como disolvente de la solución, Ethanol (10% de 50mL) con el fin de reducir la tensión superficial del agua que es 72 Nm-1, para permitir la dispersión de la solución depositada sobre el sustrato fácilmente. En una segunda etapa se han dopado pel¿culas delgadas de SnS con algún elemento en la tabla de Mendeleiev para modificar las propiedades f¿sicas y qu¿micas de las pel¿culas. Los elementos químicos utilizados fueron: Plata, Aluminio y Hierro. Se han utilizado varias técnicas de caracterización: - Difracción de rayos X (XRD) para la estructura cristalina de las películas - Espectroscopía Raman para la calidad de las películas - Microscopía electrónica de barrido (SEM) para morfología superficial - Microscopía de Fuerza Atómica (AFM) para topografía de superficie - Análisis dispersivo de energía de rayos X (EDAX) adjunto a SEM para la composición de la película - Espectrofotometría óptica para la transmisión y la determinación del gap - Método de 4 puntas para medición de resistividad del SnS dopado -Mott-Schottky para determinar el tipo de semiconductor y la concentración de portadores Los principales resultados obtenidos en esta tesis pueden resumirse como sigue: -Las películas delgadas mono-sulfuro (SnS) deben depositarse sobre un sustrato de vidrio con [S] / [Sn] igual a una (1) y la temperatura del sustrato igual a 350 ° C para obtener películas densas, bien cubiertas y homogéneas sin agujeros Y grietas. Distancia entre la boquilla al sustrato 25 cm, volumen pulverizado 5 ml, presión de aire 0,7 bar y velocidad de pulverización de 1,5 ml / min. - Para películas dopadas por Plata y Aluminio, todas las películas son estructura ortorrómbica con (111) como pico principal. La intensidad del pico principal aumenta cuando el porcentaje de elemento dopante aumenta en la solución inicial sin ninguna fase secundaria para el dopaje con Al y con Ag8SnS6 y Ag para el dopaje Ag. - El análisis de SEM y AFM demuestra que el elemento dopante Ag no tiene efecto en la morfología y ni en la topografía mientras que el dopaje Al actúa sobre la morfología superficial produciendo una morfología que presenta muchos agujeros para muestras dopadas de 3% a 7%. - EDAX destaca un aumento de Ag en películas cuando la cantidad de Ag aumenta en la solución con S/ Sn¿0,98 cerca de 1 al 5% de porcentaje de dopado de Ag donde como para el dopaje EDAX destaca la mejora de la estequiometría con un aumento del porcentaje de Al Atómica en películas cuando la concentración de Al aumenta en la solución inicial con S / Sn = 0, 99 al 10%. - La resistividad de las muestras dopadas con Ag y Al aumenta con la concentración de dopado y se observa un aumento del gap óptico de 1.66eV a 1.70eV para SnS dopado por Ag y SnS dopado por Al, respectivamente. / ß-In2S3 thin films deposited by Chemical Spray Pyrolysis technique at different substrate temperatures (250 °C-300 °C-350 °C) showed well crystallized thin films with (0 0 12) as preferred direction perpendicular to the plane containing the surface of glass substrate. SEM images showed dense, uniform, well-covered layers that adhere well to substrates and no crack and void space were noted for all substrate temperatures. Microanalysis X confirms the presence of In and S elements with good stoichiometry after vacuum annealing for 30 minutes. Raman spectroscopy analysis confirms ß-In2S3 phase with more prominent modes after vacuum annealing. We also noted a reduction in the gap energies after annealing for films prepared at 250 °C and 350 °C substrate temperatures while for those prepared at 300 °C, the energy of the gap remains stable. Tin mono-sulfide (SnS) thin films must be deposited onto glass substrate with [S]/[Sn] ratio equal to one (1) and substrate temperature equal to 350 °C to obtained dense, well-covered, and homogeneous films without pinholes and cracks. Distance between nozzle to substrate is kept to 25cm, sprayed volume 5mL, air pressure 0.7bar and spray rate 1.5 mL/min. Films doped with Silver (Ag) and Aluminum (Al) were all orthorhombic structure with (111) as main peak. The intensity of main peak increased when the percentage of dopant element increased in the initial solution without any secondary phase for Al-doping films and with Ag8SnS6 and Ag for Ag-doping ones. SEM and AFM analysis showed that Ag-doping element had no effect in the morphology and the topography while Al-doping affected the surface morphology with "fishing net" like morphology with lots of holes for samples doped from 3% to 7%. EDS highlighted an increase of Ag in films when its amount increased in the solution with S/Sn¿0.98 near to 1 at 5% of Ag-doping percentage where as for Al-doping EDS highlighted improvement of stoichiometry with an increase of Al percentage atomic in films when Al concentration increased in the initial solution with S/Sn¿0.99 at 10%. Electrical and energy band gap measurement showed a decrease of resistivity when Ag and Al percentages increased in the solution to reach relatively low resistivity of 108¿.cm and 170¿.cm at 10% for both, and an increased of energy band gap when the Ag and Al-doping elements increased in the solution with 1.66eV and 1.70eV for SnS doped with Ag and SnS doped with Al, respectively. Spray pyrolyzed SnS thin films doped with indium were studied using various optical and electrical techniques. Structural analysis shows that all films crystallize in orthorhombic structure with (111) as a preferential direction without secondary phases. Doping of SnS layers with indium results in better morphology with increased grain size. Absorption measurements indicate dominant direct transition with energy decreasing from around 1.7 eV to 1.5 eV with increased indium supply. Apart from direct transition, an indirect one, of energy of around 1.05 eV, independent on indium doping was identified. The photoluminescence study revealed two donors to acceptor transitions between two deep defect levels and one shallower with energy of around 90 meV. The observed transitions did not depend significantly on In concentration. The conductivity measurements reveal thermal activation of conductivity with energy decreasing from around 165 meV to 145 meV with increased In content. Finally, we were investigated the J-V characteristics of FTO/CdS/SnS,FTO/ZnO/CdS/SnS, FTO/ZnO:Al/CdS/SnS, FTO/ZnO:Al/SnS and FTO/In2S3/SnS solar cells and we found that efficiencies are very low due probably to the recombination at the junction, grain boundaries, etc. / L'objectiu d'aquesta tesi és la síntesi de pel·lícules primes de SnS utilitzant tècniques de baix cost per tal de fabricar cèl·lules solars amb alta eficiència. La nostra contribució rau en estudiar nous materials susceptibles de ser utilitzats per a aplicacions fotovoltaiques, i que puguin ser preparats amb tècniques de baix cost com la tècnica de Spray Piròlisis Químic (CSP) i caracteritzar alguns materials triats per a aquest fi, com ara el Sulfur de estany (SnS). S'han fabricat cèl·lules solars a partir de la disposició de capes: Mo/SnS /Tampó/i-ZnO/ZnO: Al/ Metall. Les capes de per al bufer intermèdi has sigut de In2S3 i CdS. En la primera etapa hem procedit a l'optimització dels paràmetres de deposició de pel·lícules primes de SnS usant la tècnica CSP. -Variació de la relació [S] / [Sn]. -Variació de la temperatura Ts del substrat. -Variació de la naturalesa del substrat utilitzant substrat com: vidre simple, òxid d'estany d'indi (ITO) i vidre recobert de molibdè. Les fonts de productes químics i dissolvents utilitzats han sigut; Clorur d'estany per a l'estany (Sn), thiourea per sofre (S). Aigua destil·lada com a dissolvent de la solució. Ethanol (10% de 50ml) per tal de reduir la tensió superficial de l'aigua que és 72 Nm-1, per a permetre la dispersió de la solució dipositada fàcilment sobre el substrat. En una segona etapa s'han dopat pel.lícules primes de SnS amb algun element en la taula de Mendeleiev per modificar les propietats físiques i químiques de les pel.l¿cules. Els elements químics utilitzats són: Plata (Ag+), alumini (Al3+), Ferro (Fe2+), Coure (Cu2+) i Antimoni (SB3+) com a font de nitrat de plata (AgNO3), Clorur d'alumini (AlCl3) (FeCl2·4H2O ), Clorur de Coure (CuCl2 i Clorur de Antimoni (SbCl3). S'han utilitzat diverses tècniques de caracterització: - Difracció de raigs X (XRD) per a l'estructura de les pel·lícules i cristal - Raman Spectroscopy per a la qualitat de les pel·lícules - Microscòpia electrònica de rastreig (SEM) per morfologia superficial - Microscòpia de Força Atòmica (AFM) per topografia de superfície - Anàlisi dispersiu d'energia de raigs X (EDAX) adjunt a SEM per a la composició de la pel·lícula -Espectrofotometría per a la transmissió i el mesurament de la banda d'energia utilitzant la trama de Tauc - Tècnica de punta-sonda per a mesurament de resistivitat amb dopat SnS -Mott-Schottky per determinar el tipus de semiconductor i la concentració de portadors Els principals resultats obtinguts en aquesta tesi poden resumir així: -Les pel·lícules primes mico-sulfur (SnS) han de dipositar-sobre un substrat de vidre amb [S]/[Sn] igual a una (1) i la temperatura del substrat igual a 350 °C per obtenir pel·lícules denses, ben cobertes i homogènies sense forats I esquerdes. Distància entre el filtre al substrat 25 cm, volum polvoritzat 5 ml, pressió d'aire 0,7 bar i velocitat de polvorització de 1,5 ml / min. Per pel·lícules dopades per Plata i alumini, totes les pel·lícules són estructura ortorrómbica amb (111) com pic principal. La intensitat del pic principal augmenta quan el percentatge d'element dopant augmenta en la solució inicial sense cap fase secundària per al dopatge amb Al i amb Ag8SnS6 i Ag per al dopatge Ag. L'anàlisi de SEM i AFM demostra que l'element dopant Ag no té efecte en la morfologia i la topografia mentre que el dopatge en actua sobre la morfologia superficial produint una morfologia que presenta molts forats per a mostres dopades de 3% a 7%. EDAX destaca un augment de Ag en pel·lícules quan la quantitat d'Ag augmenta en la solució amb S / Sn¿0,98 prop d'1 a 5% de percentatge de dopatge d'Ag on com per al dopatge EDAX destaca la millora de l'estequiometria amb un augment del percentatge d'al Atòmica en pel·lícules quan la concentració d'al augmenta en la solució inicial amb S / Sn = 0,99 al 10%. / Sall, T. (2017). Preparation and Characterization of SnS thin films by Chemical Spray Pyrolysis for fabrication of solar cells [Tesis doctoral]. Universitat Politècnica de València. https://doi.org/10.4995/Thesis/10251/95412

A rich variety of phases can exist in quantum systems. For example, the fractional quantum Hall states have persistent topological characteristics that derive from strong interaction. This thesis uses the exact diagonalization method to investigate quantum lattice models with strong interaction. Our research topics revolve around quantum phase transitions between novel phases. The goal is to find the best schemes for realizing these novel phases in experiments. We studied the fractional Chern insulator and its transition to uni-directional stripes of particles. In addition, we studied topological Mott insulators with spontaneous time-reversal symmetry breaking induced by interaction. We also studied emergent kinetics in one-dimensional lattices with spin-orbital coupling. The exact diagonalization method and its implementation for studying these systems can easily be applied to study other strongly correlated systems. / PHD / Topological quantum states are a new type of quantum state that have properties that cannot be described by local order parameters. These types of states were first discovered in the 1980s with the integer quantum Hall effect and the fractional quantum Hall effect. In the 2000s, the predicted and experimentally discovered topological insulators triggered studies of new topological quantum states. Studies of strongly correlated systems have been a parallel research topic in condensed matter physics. When combining topological systems with strong correlation, the resulting systems can have novel properties that emerge, such as fractional charge. This thesis summarizes our work that uses the exact diagonalization method to study topological states with strong interaction.

Submitted by Irene Nascimento (irene.kessia@ufpe.br) on 2017-04-17T18:48:07Z No. of bitstreams: 2 license_rdf: 1232 bytes, checksum: 66e71c371cc565284e70f40736c94386 (MD5) Dissertação Mestrado.pdf: 3421668 bytes, checksum: 4a6d6f2568841028e0b66b952f2d15ba (MD5) / Made available in DSpace on 2017-04-17T18:48:07Z (GMT). No. of bitstreams: 2 license_rdf: 1232 bytes, checksum: 66e71c371cc565284e70f40736c94386 (MD5) Dissertação Mestrado.pdf: 3421668 bytes, checksum: 4a6d6f2568841028e0b66b952f2d15ba (MD5) Previous issue date: 2016-08-30 / Este trabalho é uma extensão de uma modelagem tight−binding de estados de Wannier com interação coulombiana de screening para a descrição de elétrons correlacionados nas camadas de CuO2 do La2CuO4. Na condição de banda semicheia e temperatura T = 0 K, esta modelagem é capaz de predizer um estado fundamental antiferromagnético isolante e um estado excitado paramagnético com pseudo-gap, cuja natureza ainda é debatido na literatura. Esses estados são obtidos no contexto de uma solução auto-consistente tipo Hartree-Fock na modelagem de uma banda efetiva de estados de Wannier, sob condições de quebra de simetria de translações espaciais e efeito de emaranhamento (entanglement) na estrutura espinorial dos estados eletrônicos. No regime dopado com buracos, esses estados ficam degenerados num ponto crítico de concentração de buracos igual a xc = 0.2, resultando em uma transição de fase quântica de segunda ordem para um estado paramagnético. A modelagem dá assim explicação à existência detectada experimentalmente desta transição de fase. Em nosso trabalho generalizamos o termo cinético da modelagem acima mencionada através da inclusão de hopping entre segundos vizinhos, de acordo com observações experimentais. De fato, a inclusão deste novo termo cinético resulta em melhor concordância da previsão da modelagem e as observações experimentais da evolução da superfície de Fermi com dopagem de buracos. Em particular, enquanto na modelagem restrita a primeiros vizinhos não podemos conciliar a transição de fase quântica observada a xc = 0.2 com as características experimentais da evolução da superfície de Fermi, isto torna-se possível com a inclusão do hopping de segundos vizinhos com amplitude sugerida pelos resultados experimentais. / This work is an extension of a tight - binding model of states of Wannier with screened Coulomb interaction to the description of correlated electrons in the layers of CuO2 of the La2CuO4. In condition of half-filled band and temperature T = 0 K, this model is able to predict a antiferromagnetic insulating ground state and a paramagnetic excited state with pseudo-gap, which nature is still debated in the literature. These states are obtained in the context of a self-consistent solution type Hartree-Fock in the model of an effective band of the Wannier states under breaking conditions of symmetry of space translations and entanglement effect in the spinor structure of the electronic states. In scheme doped with holes, these states are degenerate at critical point of hole concentration equal to xc = 0.2, resulting in a quantum phase transition of second order to paramagnetic state. The model thus gives explanation to the existence of this experimentally detected phase transition. In our work we generalize the kinetic term of above mentioned model by inclusion of hopping between seconds neighboring, according to experimental observations. In fact, the inclusion of this new kinetic term results in better agreement of the forecast of the model and experimental observations of the evolution of the Fermi surface with holes doping. In particular, while the model is restricted to the first neighbors can not reconcile quantum phase transition observed at xc = 0.2 with the experimental characteristics of the evolution of the Fermi surface, this becomes possible with the inclusion of hopping between second neighboring with ampliude suggested by experimental results.

Orientador: Eduardo Miranda / Tese (doutorado) - Universidade Estadual de Campinas, Instituto de Física Gleb Wataghin / Made available in DSpace on 2018-08-23T18:51:04Z (GMT). No. of bitstreams: 1 SuarezVillagran_MarthaYolima_D.pdf: 7321255 bytes, checksum: d76479a0e0c1143207cb4ee380a8034d (MD5) Previous issue date: 2013 / Resumo: Estudamos nesta tese alguns aspectos da transição metal-isolante de Mott no caso desordenado. O modelo no qual baseamos nosso estudo é o modelo de Hubbard desordenado, que é o modelo mais simples a apresentar a transição metal-isolante de Mott. Analisamos esse modelo através da Teoria Dinâmica de Campo Médio Estatística (StatDMFT). Essa teoria é uma extensão natural da Teoria Dinâmica de Campo Médio (DMFT), que foi usada com relativo sucesso nos últimos anos para analisar a transição de Mott no caso limpo. Como no caso dessa última, a StatDMFT incorpora os efeitos de correlação eletrônica apenas nos seus aspetos locais. A desordem é tratada de maneira a incorporar todos os efeitos de localização de Anderson. Com essa técnica, analisamos a transição de Mott desordenada no caso bi-dimensional, usando o Monte Carlo quântico para resolver os problemas de impureza única de Anderson requeridos pela StatDMFT. Encontramos as linhas espinodais nas quais o metal e o isolante deixam de ser meta-estáveis. Também estudamos os padrões espaciais das flutuações de quantidades locais, como a auto-energia e a função de Green local, e mostramos como há o aparecimento de regiões metálicas dentro do isolante e viceversa. Analisamos efeitos de tamanho finito e mostramos que, em consonância com os teoremas de Imry e Ma, a transição de primeira ordem desaparece no limite termodinâmico. Analisamos as propriedades de transporte desse sistema através de um mapeamento a um sistema de resistores aleatórios clássicos e calculamos a corrente média e sua distribuição através da transição metal-isolante. Finalmente, estudamos o comportamento da parede de domínio que se forma entre o isolante e o metal no caso limpo. Isso foi feito através de um modelo de uma cadeia unidimensional conectada a reservatórios, um metálico e um isolante, cada um em uma de suas extremidades. Nesse caso, utilizamos o método da Teoria de Perturbação Iterada para a solução dos modelos de impureza única. Encontramos o comportamento da parede como função da temperatura e das interações / Abstract: In this thesis, we studied some aspects of the Mott metal-insulator transition in the disordered case. The model on which we based our analysis is the disordered Hubbard model, which is the simplest model capable of capturing the Mott metal-insulator transition. We investigated this model through the Statistical Dynamical Mean-Field Theory (statDMFT). This theory is a natural extension of the Dynamical Mean-Field Theory (DMFT), which has been used with relative success in the last several years with the purpose of describing the Mott transition in the clean case. As is the case for the latter theory, the statDMFT incorporates the electronic correlation effects only incorporate Anderson localization effects.. With this technique, we analyzed the disordered two-dimensional Mott transition, using Quantum Monte Carlo to solve the associated single-impurity problems. We found the spinodal lines at which metal and insulator cease to be meta-stable. We also studied the spatial fluctuations of local quantities, such as the self-energy and the local Green¿s function, and showed the appearance of metallic regions within the insulator and vice-versa. We carried out an analysis of finite-size effects and showed that, in agreement with the theorems of Imry and Ma, the first-order transition is smeared in the thermodynamic limit. We analyzed transport properties by means of a mapping to a random classical resistor network and calculated both the average current and its distribution across the metalinsulator transition. Finally, we studied the behavior of the domain wall which forms between the metal and the insulator in the clean case. This was done by means of a model of a one-dimensional chain connected to two reservoirs, one metallic and the other insulating, each attached to one of the chain¿s ends. In this case, we used the Iterated Perturbation Theory technique in order to solve the associated singleimpurity problems. We then established the behavior of the domain wall width as a function of temperature and interactions / Doutorado / Física / Doutora em Ciências

Les propriétés structurales et électroniques de films ultra-minces d'alcalins (K,Cs) déposés sur un substrat de Si(111)-v3´v3R30:B ont été étudiés par diffraction d'électrons lents (LEED), spectroscopie Auger, microscopie à effet tunnel (STM) et photoemission (ARPES, XPS). Un état de surface de symétrie s-pz a été mis en évidence par photoémission résolue en angle celui-ci présentant un maximum au taux optimal. Le site d'adsorption H3 a été identifié par IV-LEED en accord avec les prédictions théoriques. Nos mesures ARPES mettent en évidence un repliement de la bande de surface, son caractère fortement isolant ainsi qu'une largeur de bande très étroite. Dans le cas des dépôts de Césium, le gap est cependant réduit et il apparaît du poids spectral au niveau de Fermi. Ces résultats sont a priori en accord avec le caractère corrélé de ces états, ceux-ci ayant été définis initialement comme des isolants de Mott. Cependant, nous mettons en évidence dans ce travail une nouvelle reconstruction 2v3´2v3 caractérisée par un quadruplement de la maille de surface et associée à un gain d'énergie des électrons participant à l'état de surface. De plus, la dépendance en température des spectres de photoémission suggèrent un fort élargissement Franck-Condon associé à un fort couplage électron-phonon. L'étude des raies de cœur par photoémission haute résolution sur la ligne CASSIOPEE (synchrotron SOLEIL) nous a permis de mettre en évidence un ordre de charge à la surface pour les deux types de reconstruction observées en LEED. Tous nos résultats expérimentaux indiquent un fort couplage avec le réseau des électrons de l'état de surface induit par les alcalins ce qui n'a jamais été reporté auparavant ni fait l'objet de prédictions. Un scénario basé sur l'établissement d'une onde de densité de charge à la surface dans la limite d'un fort couplage électron-phonon est proposé. IL est proposé que la limite de l'isolant bi-polaronique soit atteinte dans le cas des couches ultra-minces d'alcalins/Si(111) offrant ainsi la possibilité d'étudier le comportement des électrons fortement couplés au réseau en présence de corrélations électroniques sur un réseau triangulaire. / Low energy electron diffraction (LEED), Auger spectroscopy, scanning tunneling microscopy (STM) and angle-resolved photoemission (ARPES) have been used to study ultrathin films of alkali atoms deposited on Si(111)-v3´v3R30:B surface. An alkali-induced surface state of s-pz symmetry has been evidenced by photoemission being maximum close to the saturation coverage of 1/3 monolayer. A quantitative IV-LEED study evidences the H3 alkali adsorption site as predicted by ab initio calculations. High resolution ARPES data presented in this work evidence a band-folding, a large alkali-dependent semi-conducting gap and a narrow bandwidth. The Cs- induced surface band is shown to present a smaller gap together with a non-zero spectral weight at the Fermi level. These results are a priori consistent with the correlated nature of these materials, the Harrison criterion U/W>>1 being fulfilled for these half-filled surface bands. Moreover, a novel 2v3´2v3 lattice and charge ordering has been discovered below 300 K characterized by a quadrupling of the unit cell and a net energy gain for the surface band. In addition, the temperature dependence of the ARPES spectra suggests these materials are characterized by a strong electron-phonon coupling. High resolution core-levels photoemission spectroscopy recorded at the CASSIOPEE beamline (synchrotron SOLEIL) evidence a local charge ordering at surface in both phases. The corresponding band mapping agree well with the 2(v3´v3) symmetry also for both phases. All these experimental results sign a strong interplay between the charge and lattice degrees of freedom which have never been predicted for these semiconducting surfaces. Therefore, a scenario assuming a charge density wave at surface in the strong electron-phonon coupling limit is proposed. As a striking point, the bi-polaronic insulating ground state is proposed to be reached making these alkali/Si(111) semi-conducting surfaces model systems to study polaronic signatures on the physical properties of low dimensional strongly correlated materials.