Ce manuscrit de thèse présente une étude expérimentale des propriétés optiques, électroniques et structurales du diamant fortement dopé au bore. Ce semi-conducteur à large bande interdite peut être synthétisé par dépôt chimique en phase vapeur assisté par plasma micro-onde (MPCVD). Il est intrinsèquement isolant mais devient métallique, voire supraconducteur conventionnel par dopage de type p. Ce travail s'articule autour de trois grands axes :Le premier concerne le développement de l'ellipsométrie spectroscopique pour la caractérisation de couches de diamant monocristallin. Dans un premier temps, des modèles optiques ont été développés afin de déduire les épaisseurs, résistivités et concentrations de porteurs de plusieurs séries d'échantillons mesurés ex situ. Ces valeurs ont été confrontées à celles obtenues par le biais de mesures SIMS (Spectroscopie par Emission d'ion Secondaires) et de transport électronique. Une masse effective optique des porteurs a pu ainsi être évaluée. Dans un second temps, cette technique a été mise en oeuvre in situ sur le réacteur. L'influence de la température et de la géométrie de la chambre de réaction a été évaluée et des suivis de croissance en temps réel sont présentés.Le second axe porte sur la synthèse des échantillons et l'optimisation des paramètres de croissance. Dans cette partie, nous révélons la présence d'un transitoire dans l'incorporation du bore conduisant à une inhomogénéité de dopage des échantillons. Une augmentation de l'incorporation du bore avec le débit a également été observée pour la première fois. Enfin, la détérioration de la qualité cristalline du diamant, au delà d'une concentration critique d'atomes de bore, est identifiée et discutée.Le troisième et dernier axe de ces travaux de recherche, est dédié à l'investigation des propriétés électroniques du diamant fortement dopé par magnéto-transport de 300K à 50 mK. Dans un premier temps, l'importance de la mésa-structuration de croix de Hall lors des mesures de transport est mise en évidence. L'utilisation d'une géométrie « maîtrisée », permet en effet de limiter les courants parasites dus à l'inhomogénéité de dopage des couches. Nous avons ainsi pu construire un diagramme de phase différent de celui qui avait été rapporté dans la littérature. Une phase métallique et non supraconductrice a été mise en évidence pour la première fois. Une étude de la transition métal-isolant est présentée, et les exposants critiques issus de sa modélisation sont discutés. L'étude de l'état supraconducteur enfin, nous a permis d'aboutir à une nouvelle dépendance de la température de transition (Tc) avec le dopage. Cette dernière est comparée aux calculs ab initio de la littérature. Aucune réduction de la Tc avec l'épaisseur n'a en revanche été observée dans la gamme des couches synthétisées à savoir de 10 nm à 2 µm. / This PhD thesis reports on an experimental study of optical, electronic and structural properties of heavily boron-doped diamond. This wide bandgap semiconductor can be synthesized by Plasma Enhanced Chemical Vapor (MPCVD). Diamond is an insulator that may turn metallic and even superconductor (conventional) upon p-type doping.This work can be divided into three main parts :The first one involves the development of spectroscopic ellipsometry for characterizing single crystal diamond epilayers. First, optical models have been developed to derive the thickness, resistivity and carrier concentrations of several sets of samples measured ex situ. These values were then compared to those obtained through SIMS profiles (Secondary Ion Mass Spectroscopy) and transport measurements. As a result, an optical effective mass of carriers was determined. Second, this technique has been implemented to be set up in situ on the reactor. The influence of the temperature and the geometry of the growth chamber has been evaluated, and real time growth monitoring was achieved.The second part is related to the sample synthesis and optimization of growth parameters. In this section, we reveal the presence of a transient regime in the boron incorporation leading to a doping inhomogeneity. An increase of boron incorporation with the gas flow was also observed for the first time. Finally, the deterioration of the crystalline structure of diamond, above a critical dopant concentration, was identified and discussed.The third axis of this research is dedicated to the investigation of the electronic properties of heavily doped diamond by magneto-transport from 300K to 50 mK. First, the importance of the Hall bar mesa patterning for transport measurements is stressed. The use of a “controlled” geometry limited parasitic currents associated with doping inhomogeneities. Thus we could construct a new phase diagram, differing from previous reports in the literature. A metallic and non-superconducting layer has been unveiled for the first time. A study of the metal-insulator transition is reported and the critical exponents deduced from its modelling are discussed. Finally, the study of the superconducting state revealed a new dependence of the transition temperature (Tc) on doping which is compared with ab initio calculations. However, not any significant reduction of Tc was observed when the layer thickness dropped from 2 µm to 10 nm.

No description available.

Ce manuscrit présente une étude expérimentale de phase isolante non-conventionnelle, l'isolant d'Anderson, induit par le désordre, l'isolant de Mott, induit par les interactions de Coulomb, et les isolants topologiques.Dans une première partie du manuscrit, je décrirais le développement d'une méthode pour étudier la réponse de charge de nanoparticules par Microscopie à Force Electrostatique (EFM). Cette méthode a été appliquée à des nanoparticules de magnétite (Fe3O4), un matériau qui présente une transition métal-isolant, i.e. la transition de Verwey, lors de son refroidissement en dessous d'une température TV~120 K.Dans une seconde partie, ce manuscrit présente une étude détaillée de l'évolution de la densité d'états au travers de la transition métal-isolant entre un isolant de type Anderson-Mott et une phase métallique dans le matériau SrTiO3, et ceci, en fonction de la concentration de dopants, les lacunes d'oxygènes. Nous avons trouvé que dans un dispositif memoresistif de type Au-SrTiO3-Au, la concentration de dopants pouvait être ajustée par migration des lacunes d'oxygènes à l'aide d'un champ. Dans cette jonction tunnel, l'évolution de la densités d'états au travers de la transition métal-isolant peut être étudiée de façon continue. Finalement, dans une troisième partie, le manuscrit présente le développement d'une méthode pour la microfabrication d'anneaux de Aharonov-Bohm avec l'isolant topologique, Bi2Se3, déposée par épitaxie à jet moléculaire. Des résultats préliminaires sur les propriétés de transport quantique de ces dispositifs seront présentés. / This manuscript presents an experimental study of unconventional insulating phases, which are the Anderson insulator, induced by disorder, the Mott insulator, induced by Coulomb interactions, and topological insulators.In a first part of the manuscript, I will describe the development of a method to study the charge response of nanoparticles through Electrostatic Force Microscopy (EFM). This method has been applied to magnetite Fe3O4 nanoparticles, a material that presents a metal-insulator transition, i.e. the Verwey transition, upon cooling the system below a temperature Tv=120K. In a second part, this manuscript presents a detailed study of the evolution of the Density Of States (DOS) across the metal-insulator transition between an Anderson-Mott insulator and a metallic phase in the material SrTiO3 and this, as function of dopant concentration, i.e. oxygen vacancies. We found that in this memristive type device Au-SrTiO3-Au, the dopant concentration could be fine-tuned through electric-field migration of oxygen vacancies. In this tunnel junction device, the evolution of the DOS can be followed continuously across the metal-insulator transition. Finally, in a third part, the manuscript presents the development of a method for the microfabrication of Aharonov-Bohm rings with the topological insulator material, Bi2Se3, grown by molecular beam epitaxy. Preliminary results on the quantum transport properties of these devices will be presented.

J'étudie en détail la solution d'un modèle simplifié d'électrons fortement corrélés, à savoir le modèle de Hubbard dimérisé. Ce modèle est la réalisation la plus simple d'un problème de cluster DMFT. Je fournis une description détaillée des solutions dans une région de coexistence où l'on trouve deux états (méta) stables des équations DMFT, l'un métallique et l'autre isolant. De plus, je décris en détail comment ces états disparaissent à leurs lignes critiques respectives. Je clarifie le rôle clé joué par la corrélation intra-dimère, qui agit ici en complément des corrélations de Coulomb.Je passe en revue la question importante du passage continue entre unisolant Mott et un isolant Peierls où je caractérise une variété de régimes physiques. Dans un subtil changement de la structure électronique, lesbandes de Hubbard évoluent des bandes purement incohérentes (Mott) à desbandes purement cohérentes (Peierls) à travers un état inattendu au caractère mixte. Je trouve une température d'appariement singulet T* en-dessous de laquelle les électrons localisés à chaque site atomique peuvent se lier dans un singulet et minimiser leur entropie. Ceci constitue un nouveau paradigme d'un isolant de Mott paramagnétique.Enfin, je discute la pertinence de mes résultats pour l'interprétation de différentes études expérimentales sur VO₂. Je présente plusieurs arguments qui me permettent d'avancer la conclusion que la phase métallique, à vie longue (métastable) induite dans les expériences pompe-sonde, et l'état métallique métastable M₁, thermiquement activé dans des nano-domaines, sont identiques. De plus, ils peuvent tous être qualitativement décrits, dans le cadre de notre modèle, par un métal corrélé dimérisé. / We study in detail the solution of a basic strongly correlated model,namely, the dimer Hubbard model. This model is the simplest realization ofa cluster DMFT problem.We provide a detailed description of the solutions in the ``coexistentregion'' where two (meta)stable states of the DMFT equations are found, onea metal and the other an insulator. Moreover, we describe in detail howthese states break down at their respective critical lines. We clarify thekey role played by the intra-dimer correlation, which here acts in additionto the onsite Coulomb correlations.We review the important issue of the Mott-Peierls insulator crossoverwhere we characterize a variety of physical regimes. In a subtle change inthe electronic structure the Hubbard bands evolve from purely incoherent(Mott) to purely coherent (Peierls) through a state with unexpected mixedcharacter. We find a singlet pairing temperature T* below which thelocalized electrons at each atomic site can bind into a singlet and quenchtheir entropy, this uncovers a new paradigm of a para-magnetic Mottinsulator.Finally, we discuss the relevance of our results for the interpretation ofvarious experimental studies in VO₂. We present a variety of argumentsthat allow us to advance the conclusion that the long-lived (meta-stable)metallic phase, induced in pump-probe experiments, and the thermallyactivated M₁ meta-stable metallic state in nano-domains are the same.In fact, they may all be qualitatively described by the dimerizedcorrelated metal state of our model.

Dissolution of hydrogen into intermetallic compounds characteristically occurs at interstitial sites, causing little alteration to the base metal substructure but often bringing about substantial electronic and magnetic changes to the material. These hydrogen-induced alterations in the intermetallic hydrides are of interest both on a fundamental research level and in terms of technological applications; however, there exists no general theory as to how and why these alterations arise. The objective of this research is to elucidate to general effect of hydrogen on intermetallic compounds through the study of crystallographic, magnetic and electronic properties. An investigation has been carried out on the properties of three intermetallic compound - hydrogen systems of general formula ZrM₂, where M = V, Cr, Mn. All three compounds reversibly absorbed hydrogen with no change in crystal symmetry: powder diffraction studies showed that hydrogen was accommodated in interstitial sites of the existing metal sublattice via lattice expansion. The measurement of the magnetic properties of these systems was combined with the determination of conductivity and dielectric properties in order to describe the electronic e¤ects of hydrogen absorption. Despite the lack of signi…cant structural alteration in these systems, electron transfer between the metal sublattice and hydrogen may occur, as manifested in the appearance/disappearance of magnetic phenomena and the increase/decrease of electrical conductivity. Whilst the hydrogen addition in ZrM₂-H occurs simply via an expansion of the crystal structure, hydrogen does not act purely as null dilutant - there exist subtle electronic changes connected with the hydriding process as well.

In dieser Arbeit wird ein Modell für das Eu-reiche EuO formuliert. Es besteht in einer Erweiterung des Kondo-Gitter-Modells (KGM). Für das KGM existieren nur einige exakte Aussagen. In dieser Arbeit kommt eine neue hinzu, nämlich die exakte Abbildung des periodischen Anderson-Modells auf das antiferromagnetische KGM für beliebige Kopplungsstärke J. Reines EuO ist ein ferromagnetischer Halbleiter. Eu-reiches EuO zeigt einen gewaltigen Metall-Isolator-Übergang in der Nähe der Curie-Temperatur mit einem Sprung im Widerstand von bis zu 13 Größenordnungen. Das ist der größte Sprung im Widerstand, der jemals in der Natur beobachtet wurde. Wir reproduzieren diesen Sprung theoretisch mit der Kubo-Formel. Wir erzielen sehr gute Fits bereits in einer nicht vollständig selbstkonsistenten Theorie, bei der die Magnetisierung der Eu-Spins einer Brillouin-Funktion entnommen ist. In einer vollständig selbstkonsistenten Theorie bestimmen wir die Magnetisierung, die Curie-Temperatur, den spezifischen Widerstand und andere Transporteigenschaften. Wir berechnen Größen wie die elektronische Wärmeleitfähigkeit und die Thermokraft, für die weniger experimentelle Daten zum Vergleich vorhanden sind. Nichtsdestoweniger erscheinen z.B. die Rechnungen für die thermische Leitfähigkeit vertrauenswürdig, da das Wiedemann-Franz-Verhältnis mit der elektrischen Leitfähigkeit einen vernünftigen Wert liefert. Die Leitungselektronenzahl des Eu-reichen EuO kommt aus der Theorie unabhängig von der Leitfähigkeit heraus. Daher können wir aus der Leitfähigkeit und der Leitungselektronenzahl die durchschnittliche Drude-Mobilität (oder Streuzeit) berechnen. Diese Größe hat für höhere Impurity-(Sauerstoff-Leerstellen)-Konzentrationen einen Sprung in der Nähe der Curie-Temperatur von bis zu zwei Größenordnungen in Übereinstimmung mit dem Experiment. / In this thesis a model is formulated for Eu-rich EuO. It consists in an extension of the Kondo lattice model (KLM). For the KLM only a few exact statements exist. To those we add a new one, namely the exact mapping of the periodic Anderson model on the antiferromagnetic KLM for arbitrary coupling constant J. Pure EuO is a ferromagnetic semiconductor. Eu-rich EuO exhibits a huge metal--insulator transition near the Curie temperature with a jump in resistivity of up to 13 orders of magnitude. It is the biggest jump in resistivity ever observed in nature. We theoretically reproduce this jump. We achieve very good fits already within a not fully self-consistent theory where the magnetization of the Eu spins is taken from a Brillouin function. In a fully self-consistent theory we determine the magnetization, the Curie temperature, the resistivity and other transport properties. We calculate quantities like the electronic thermal conductivity and the thermopower, for which there are less experimental data to compare with. Nevertheless, e.g. the calculations for the thermal conductivity seem reliable since the Wiedemann-Franz ratio with the electrical conductivity gives a reasonable result. The conduction-electron number of Eu-rich EuO comes out of the theory independently of the conductivity. So we can calculate from the conductivity and the conduction-electron number the average Drude mobility (or scattering time). This quantitiy has a jump near the Curie temperature of up to two orders of magnitude for higher impurity (oxygen vacancy) concentrations in agreement with the experiment.

No description available.

Transition metal and related compounds have been extensively studied over the past several decades. These investigations revealed a wide range of behavior, encompassing colossal magnetoresistance (CMR), high-TC superconductivity, and magnetic semiconductivity, all of which continue to present fundamental challenges to the understanding of such phenomena. There is, however, a close correlation between such characteristics and the appearance of magnetic order. This correlation underlies the present study, which focuses on the magnetic and transport behavior of various Manganese (Mn), Iron (Fe) and Cobalt (Co) containing materials, with particular emphasis on the nature of the magnetic order they display and the critical exponents that characterize the accompanying phase transition. The magnetic and transport properties of two specific systems will be covered: first various doped manganites from the series (La,Pr)1-x(Ca,Ba)xMnO3, and second the magnetic semiconductors Fe0.8Co0.2Si and Ga0.98Mn0.02As. In the manganites, the influence of doping on; (i) the evolution of the metal-insulator transition (MIT) with composition; (ii) the universality class of the magnetic critical behavior associated with the paramagnetic to ferromagnetic transition, which occurs in the vicinity of a MIT with which CMR is associated; (iii) the mechanisms underlying ferromagnetism across the MIT; (iv) the correlation between the appearance of a Griffiths-like phase and CMR, and (v) the origin of Griffiths-like phase have been investigated. Four different systems have been studied: La1-xCaxMnO3 (0.18 ≤ x ≤ 0.27), La1-xBaxMnO3 (x ≤ 0.33), (La1-yPry)0.7Ca0.3Mn16/18O3 (y ≤ 0.85), and Pr1-xCaxMnO3 (x = 0.27, 0.29). In Fe0.8Co0.2Si and Ga0.98Mn0.02As, the scaling between magnetization and conductivity has been the subject of ongoing debate. In bulk Fe0.8Co0.2Si, a novel scaling between the anomalous Hall effect (AHE) and the magnetization enables the anomalous Hall coefficient to be accurately determined. In turn, this enables the universality class for the transition to ferromagnetism to be established independently from the anomalous Hall conductivity. In an epitaxial (metallic) Ga0.98Mn0.02As microstructure, the magnetization has been indirectly determined from the AHE. Subsequent analysis yields magnetic critical exponents consistent with the Mean-Field model, direct support for which had previously been lacking.

Transition metal and related compounds have been extensively studied over the past several decades. These investigations revealed a wide range of behavior, encompassing colossal magnetoresistance (CMR), high-TC superconductivity, and magnetic semiconductivity, all of which continue to present fundamental challenges to the understanding of such phenomena. There is, however, a close correlation between such characteristics and the appearance of magnetic order. This correlation underlies the present study, which focuses on the magnetic and transport behavior of various Manganese (Mn), Iron (Fe) and Cobalt (Co) containing materials, with particular emphasis on the nature of the magnetic order they display and the critical exponents that characterize the accompanying phase transition. The magnetic and transport properties of two specific systems will be covered: first various doped manganites from the series (La,Pr)1-x(Ca,Ba)xMnO3, and second the magnetic semiconductors Fe0.8Co0.2Si and Ga0.98Mn0.02As. In the manganites, the influence of doping on; (i) the evolution of the metal-insulator transition (MIT) with composition; (ii) the universality class of the magnetic critical behavior associated with the paramagnetic to ferromagnetic transition, which occurs in the vicinity of a MIT with which CMR is associated; (iii) the mechanisms underlying ferromagnetism across the MIT; (iv) the correlation between the appearance of a Griffiths-like phase and CMR, and (v) the origin of Griffiths-like phase have been investigated. Four different systems have been studied: La1-xCaxMnO3 (0.18 ≤ x ≤ 0.27), La1-xBaxMnO3 (x ≤ 0.33), (La1-yPry)0.7Ca0.3Mn16/18O3 (y ≤ 0.85), and Pr1-xCaxMnO3 (x = 0.27, 0.29). In Fe0.8Co0.2Si and Ga0.98Mn0.02As, the scaling between magnetization and conductivity has been the subject of ongoing debate. In bulk Fe0.8Co0.2Si, a novel scaling between the anomalous Hall effect (AHE) and the magnetization enables the anomalous Hall coefficient to be accurately determined. In turn, this enables the universality class for the transition to ferromagnetism to be established independently from the anomalous Hall conductivity. In an epitaxial (metallic) Ga0.98Mn0.02As microstructure, the magnetization has been indirectly determined from the AHE. Subsequent analysis yields magnetic critical exponents consistent with the Mean-Field model, direct support for which had previously been lacking.

The vanadium dioxide (VO2) shows a metal-insulator transition (MIT) near the room temperature with huge changes in its electrical and optical behavior. Both the electrical and optic properties, and even the transition temperature, depend on the morphologic characteristics of the metal. In this work, vanadium oxide nanolayers were deposited onto glass substrate by reactive magnetron sputtering. The aim was to obtain the best deposition parameters, like substrate temperature (Ts) and oxygen partial pressure (PO2), for the VO2M1 phase synthesis. Samples deposited with oxygen partial pressures ranging from 10 to 20% of the total pressure, and Ts=400°C, have shown metal insulator transition when submitted to a 550°C ex-situ thermal treatment. The analysis of the x-ray diffraction spectra has shown that all the samples were formed simultaneously by more than one phase of vanadium oxides. Moreover, we identify a reciprocal correspondence between the 2q = 27,8° peak, corresponding to (011) plan in VO2M1, and the MIT transition. The measured resistance in samples with VO2M1, in the temperature range of 25 to 100°C, showed variations of almost three orders of magnitude. The transition critical temperature took place between 59 and 82°C and the hysteresis loops width ranged between 9 and 13°C / O dióxido de Vanádio (VO2) apresenta uma transição metal isolante (MIT) próxima da temperatura ambiente com uma grande variação em suas propriedades elétricas e ópticas. Tanto as propriedades elétricas e ópticas quanto a própria temperatura de transição dependem das características morfológicas do material. Neste trabalho, nano-camadas de óxido de Vanádio foram produzidas sobre substratos de vidro pela técnica de magnetron sputtering reativo, visando determinar os parâmetros de deposição, em especial a temperatura do substrato (Ts) e pressão parcial de Oxigênio (PO2), adequadas para a obtenção da fase VO2M1. Amostras depositadas com pressões parciais de Oxigênio entre 10 e 20% da pressão total e Ts=400°C apresentaram MIT quando submetidas a tratamentos térmicos ex-situ a 550°C. A análise dos espectros de difração de raios-x mostrou que houve formação de mais de uma fase simultaneamente em todas as amostras, no entanto há uma correspondência recíproca entre o pico de difração de raios-x em 2q = 27,8° , correspondente ao plano (011) do VO2M1, e a transição MIT na resistividade. As medidas de resistência em função da temperatura, realizadas entre 25 e 100°C, mostraram, nas amostras com VO2M1, transição com variação na resistência em até três ordens de grandeza com temperaturas críticas entre 59 e 82°C e curvas de histerese com larguras entre 9 e 13°C