Cette thèse présente une étude de transport électronique dans des gaz d'électrons bidimensionnels sous champ magnétique intense (60T). La première partie est dédiée au gaz d'électrons formé à l'interface entre deux isolants de bandes LaAlO3/SrTiO3. Sur la plage de champ magnétique exploré, la non-linéarité de la résistance de Hall permet d'établir un régime de conduction multi-bande. Une majorité des porteurs de charge de faible mobilité (µ ~100 cm2/Vs) occupe une bande tandis qu'une minorité de porteurs de haute mobilité (µ>1000 cm2/Vs) occupent au moins deux autres bandes de conduction. La présence d'oscillations de Shubnikov-de Haas à très basse température (450mK) est associée aux porteurs de haute mobilité. La fréquence et l'amplitude des oscillations sont profondément modifiées lorsque la densité de porteurs est modulée par couplage électrostatique. Cette étude laisse entrevoir un système électronique complexe, encore peu exploré et dans lequel un nombre important de paramètres (conditions de croissance, densité de porteurs ...) sont susceptibles d'affecter les propriétés de transport électronique. La deuxième partie est consacrée à l'étude de films inhomogènes de graphène issus d'un dépôt chimique en phase vapeur. Deux échantillons aux propriétés électroniques radicalement différentes ont été étudiés. L'un d'entre eux est constitué d'un ensemble de grains de graphène multi-feuillets fortement couplés les uns aux autres. De larges oscillations de la magnéto-résistance sont observées sous champ magnétique intense, présentant un caractère pseudo-périodique en fonction du facteur de remplissage. Cette observation suggère un régime de transport dans lequel la formation des niveaux de Landau est propre à chaque "grains" de graphène multi-couche, prévenant ainsi l'établissement du régime d'effet Hall quantique sans pour autant détruire la quantification du spectre énergétique en niveaux discrets dans la réponse globale de l'échantillon. Dans un autre échantillon, la présence d'un désordre fort localise la fonction d'onde au niveau des impuretés ou des grains de graphène multi-couche. A basse température, la conductivité est nulle (caractère isolant) tant que la tension de polarisation ne dépasse pas un certain seuil. Dans ce régime de transport, la magnéto-résistance positive observée expérimentalement possède la forme fonctionnelle du modèle VRH (Variable Range Hopping), impliquant le confinement magnétique des fonctions d'onde électroniques. La troisième partie est consacrée à la recherche des états conducteurs de surface dans les isolants topologiques, en particulier les composés Bi2Se3 et Bi2Te3. L'existence de ces états électroniques aux propriétés particulières a été prédite par de nombreuses études théoriques et confirmée expérimentalement par ARPES. Leur mise en évidence par transport électronique reste cependant controversée. Nous avons souhaité utiliser un champ magnétique intense pour tenter de révéler ces états de surface à travers l'observation d'oscillations de Shubnikov-de Haas à très basse température. Bien que les résultats obtenus n'aient pas permis d'apporter une preuve irréfutable du phénomène recherché, ces derniers seront commentés au regard de la littérature existante. / This PhD thesis focuses on electronic transport properties of two-dimensional electron gases (2DEG) under high magnetic field (60T). The first part is dedicated to the 2DEG formed at the interface between two band insulators, namely LaAlO3/SrTiO3. In the range of available magnetic field, the nonlinearity of the Hall resistance reveals a multi-band conduction system. We have found that a majority of charge carriers with low mobility (µ ~100 cm2/Vs) occupies one conduction band and a minority of high mobility carriers (µ> 1000 cm2/Vs) occupies at least two conduction bands. The presence of Shubnikov-de Haas oscillations at very low temperature (450mK) is mostly associated with the high mobility carriers. The frequency and amplitude of the oscillations are substantially modified when the carrier density is modulated by electrostatic coupling, suggesting a complex electronic system whose transport properties are strongly influenced by many external parameters (growth conditions, carrier density, temperature, quality of the interface, etc). The second part is devoted to the study of inhomogeneous graphene films deposited by chemical vapor deposition. Two samples with radically different electronic properties were studied. One of them consists of a random array of few-layer-graphene grains strongly coupled to each other. Large oscillations in the magneto-resistance are observed in high magnetic field. These oscillations are pseudo-periodic as a function of the filling factor suggesting the onset of Landau level quantization particular to each grain which, subsequently, prevents the establishment of the quantum Hall regime. In another sample, the presence of strong disorder localizes the electronic wave function close to impurities or grains of multi-layer graphene. The transport regime can be described by a model of thermally activated electron hopping. At low temperatures, the conductivity is zero (insulating behaviour) provided the bias voltage does not exceed a certain threshold. Once this threshold is reached, the charge transport is well described by a model which considers an array of weakly (capacitive) coupled conducting islands. The experimental positive magneto-resistance in high magnetic field satisfies the predictions of the VRH model (Variable Range Hopping) involving magnetic-induced shrinkage of the electronic wave functions, in consistency with the low temperature charge localization regime. The third part is devoted to the search for the surface states in topological insulators, especially in the Bi2Se3 and Bi2Te3 compounds. The existence of such surface states with special electronic properties was predicted by many theoretical studies and experimentally confirmed by Angle Resolved Photo Emission Spectroscopy. However, signatures of surface conducting states probed by electronic transport remain controversial. In this perspective, we took advantage of very high magnetic field to investigate on surface state induced Shubnikov-de Haas oscillations at very low temperature. Although the results did not provide convincing evidence of the expected phenomena, they are discussed in the context of the existing literature and pave the way for further researches.

Cette thèse s'intéresse à l'étude de la supraconductivité bidimensionnelle à l'interface entre les oxydes LaAlO3 et SrTiO3 contrôlée par effet de champ électrique. Lorsqu'on fait croître une couche mince de quelques mailles atomiques de LaAlO3 sur un substrat de SrTiO3, l'interface devient conductrice, et même supraconductrice au-dessous de 300mK, bien que ces deux oxydes de structure pérovskite soient des isolants. Il se forme ainsi un gaz bidimensionnel d'électrons de haute mobilité, dont les propriétés - supraconductivité et fort couplage spin-orbite de type Rashba - peuvent être contrôlées par effet de champ électrique à l'aide d'une Back Gate. Nous avons étudié cette supraconductivité bidimensionnelle par trois approches expérimentales différentes : l'étude de la transition supraconductrice en température à l'aide du modèle de Berezinskii-Kosterlitz-Thouless incluant une distribution inhomogène de rigidité ; l'analyse par le groupe de renormalisation de la transition de phase quantique supraconducteur-isolant induite par un champ magnétique perpendiculaire à l'interface selon le modèle de Spivak, Oreto et Kivelson ; et enfin l'étude de l'hystérèse du courant critique ainsi que de sa nature probabiliste dans le cadre du modèle RCSJ. Nous proposons donc de considérer l'interface comme un réseau de flaques supraconductrices couplées par effet Josephson à travers un gaz 2D métallique, dont la transition est régie par le modèle XY des fluctuations de phase. Enfin, nous avons démontré pour la première fois la possibilité de contrôler les propriétés du gaz 2D à l'aide d'une Top Gate, et comparé les effets des deux grilles (Top ou Back Gate). / In this PhD work, we study the field-effect modulated two-dimensional superconductivity at the LaAlO3/SrTiO3 oxides hetero-interface. When one grows epitaxially a few unit cells thin film of LaAlO3 on a SrTiO3 substrate, the interface becomes conducting, and even superconducting below 300mK, although these two perovskite oxides are insulators. The properties of this high-mobility two-dimensional electron gas – superconductivity and strong Rashba-type spin-orbit coupling - can be field-effect modulated by the mean of a Back Gate. We have investigated this two-dimensional superconductivity through three different experimental approaches : the temperature-driven transition with the Berezinskii-Kosterlitz-Thouless model including an inhomogeneous distribution of rigidity ; the finite-size scaling analysis of the superconductor-to-insulator quantum phase transition induced by a perpendicular magnetic field using the model developed by Spivak, Oreto and Kivelson ; and finally the measure of the hysteretic and stochastic properties of the critical current in the framework of the RCSJ model. We hence propose to consider this 2D electron gas as an inhomogeneous network of superconducting puddles coupled to one another by Josephson effect through a normal metallic matrix, which transition is dominated by the XY model of the phase fluctuations. Finally, we demonstrated for the first time the possibility of Top Gated-control of this interface, and we investigated the compared effects of Top and Back Gating.

La mise en évidence d'une conductivité métallique à l'interface entre deux oxydes isolants, le SrTiO3 et le LaAlO3, a ouvert un champ nouveau pour l'électronique tout oxyde (A. Ohtomo & H. Y. Hwang, Nature 427, 2004). Au-delà du fort potentiel applicatif de cette découverte, par exemple pour l'électronique de faible puissance, de nombreuses questions restent posées sur les propriétés de ces interfaces et les différents moyens de les contrôler. L'apparition de la conductivité à l'interface LaAlO3 / SrTiO3 est attribuée à la survenue d'une reconstruction électronique au-dessus d'une épaisseur critique de 4 cellules unités (u.c.) de LaAlO3, visant à compenser la discontinuité de charge à cette interface entre matériaux polaire (LaAlO3) et non polaire (SrTiO3). En plus de cet effet, qui requiert une interface d'excellente qualité, divers paramètres sont susceptibles d'affecter les propriétés de cette interface et un effort de recherche très important porte sur le contrôle et l'amélioration de ces propriétés par des moyens tels que le changement de la nature du substrat, l'application d'un champ de contraintes ou l'introduction de légères modifications chimiques dans la couche ou à l'interface. Ce travail de thèse participe à cet effort en explorant les propriétés de transport et la structure fine des interfaces LaAlO3 / SrTiO3 dopées avec des atomes de métaux de transition. Il est centré sur la fabrication et l'étude d'interfaces LaAlO3 / SrTiO3 dopées avec des atomes d'iridium ou de cobalt. La croissance de nanostructures de haute qualité, typiquement LaAlO3 (5 u.c.) / SrTiO3 dopé (1 u.c.) / SrTiO3 (substrat), a été effectuée dans un bâti de dépôt laser pulsé (PLD) équipé d'un RHEED in situ. L'effet des dopants Ir ou Co sur les propriétés de transport et sur la structure électronique et atomique de l'interface LaAlO3 / SrTiO3 a été analysé en fonction du niveau de dopage grâce à une combinaison de différentes méthodes expérimentales et de calculs DFT. En particulier, des investigations par des techniques avancées comme la diffraction de photoélectrons sur synchrotron (XPD) et la microscopie électronique de résolution atomique en mode STEM-HAADF ont été mises en œuvre pour sonder la structure locale à l'interface et quantifier le niveau de déformation dans la couche LaAlO3. La structure électronique a été étudiée par spectroscopie de perte d'énergie électronique dans un STEM. Les résultats montrent qu'il est possible d'induire des changements dans les propriétés des interfaces LaAlO3 / SrTiO3 en dopant la surface de SrTiO3 avec un dopant et une concentration appropriés. En particulier, les effets du niveau de dopage sur la déformation élastique et les distorsions locales dans les couches LaAlO3 et ses conséquences sur les propriétés mesurées sont décrits. / The demonstration in 2004 of a metallic conductivity at the interface between two insulating oxides, SrTiO3 and LaAlO3, opened a new field for all-oxide electronics (A. Ohtomo & H. Y. Hwang, Nature 427, 2004). Beyond the important applicative potential of this discovery for multifunctional and low power electronics, many questions remain about the properties of such interfaces and the different ways to control them. The occurrence of a conductive behaviour of the LaAlO3 / SrTiO3 interface is attributed to the advent of an electronic reconstruction above a critical thickness of 4 unit cells (u.c.) of LaAlO3, in order to compensate the charge discontinuity at the interface between a polar (LaAlO3) and a non-polar (SrTiO3) materials. In addition to this effect, which implies an interface of excellent quality, various parameters are likely to affect the properties of this interface, and a major research effort aims to control and improve these properties by ways such as the change in the nature of the substrate, the application of a stress field or the introduction of slight chemical modifications in the layer or at the interface. This thesis participates to this effort by exploring the transport and structural behaviour of LaAlO3 / SrTiO3 interfaces doped with transition metal atoms. It focuses on the fabrication and study of LaAlO3 / SrTiO3 interfaces doped with iridium or cobalt atoms. High quality nanostructures, typically LaAlO3 (5 u.c.) / doped-SrTiO3 (1 u.c.) / SrTiO3 (substrate), were grown by pulsed laser deposition (PLD) equipped with in-situ RHEED. The effect of Ir or Co dopants on both the transport properties and the electronic and atomic structure of the LaAlO3 / SrTiO3 interface was analysed as a function of the doping level thanks to a combination of different experimental methods and DFT calculations. In particular, advanced investigations by hard X-ray photoelectron diffraction on a synchrotron facility and by atomically resolved high angle annular dark field- scanning transmission electron microscopy (HAADF-STEM) were implemented to probe the local structure at the interface and quantify the level of strain in the LaAlO3. The electronic structure was investigated by electron energy loss spectroscopy in a STEM. Our results show that it is possible to induce changes in the properties of the LaAlO3 / SrTiO3 interfaces by doping the SrTiO3 surface with suitable dopant and concentration. In particular, effects of the doping level on the elastic deformation and the local distortions in the LaAlO3 layers and its consequences on the measured properties are described.

The properties of bulk 3D materials of metals or semiconductors are manifested with various length scales(e.g., Bohr excitonic radius, magnetic correlation length, mean free path etc.) and are important in controlling their properties. When the size of the material is smaller than these characteristics length scales, the confinement effects operate reflecting changes in their physical behavior. Materials with such confinement effects can be designated as low dimensional materials. There are exceedingly large numbers of low dimensional materials and the last half a century has probably seen the maximum evolution of such materials in terms of synthesis, characterization, understanding and modification of their properties and applications. The field of” nanoscience and nanotechnology”, have become a mature field within the last three decades where, for certain application, synthesis of materials of sizes in the nanometer range can be designed and controlled. Interface plays a very important role in controlling properties of heterogeneous material of every dimensionality. For example, the interface forms in 2D thin films or interface of heterogeneous nanoparticles(0D). In recent times, a large number of remarkable phenomena have triggered understanding and controlling properties arises due to nature of certain interface. In the field of nanoparticles, it is well known that the photoluminescence property depends very strongly on the nature of interface in heterostructured nanoparticles. In the recent time a large variety of heterostructured nanoparticles starting from core-shell to quantum dot-quantum well kind has been synthesized to increase the photoluminescence efficiency up to 80%. Along with improvement of certain properties due to heterostructure formation inside the nanoparticles, the techniques to understand the nature of those interfaces have improved side by side. It has been recently shown that variable energy X-ray Photoemission Spectroscopy (XPS) can be employed to understand the nature of interfaces (internal structure) of such heterostructure nanoparticles in great detail with high accuracy. While most of the previous studies of variable energy XPS, uses photonenergies sensitive to smaller sized particle, we have extended the idea of such nondestructive approach of understanding the nature of buried interfaces to bigger sized nanoparticles by using photon energy as high as 8000eV, easily available in various 3rd generation synchrotron centers. The nature of the interface also plays an important role in multilayer thin films. Major components of various electronic devices, like read head memory devices, field effect transistors etc., rely on interface properties of certain multilayer thin film materials. In recent time wide range of unusual phenomenon such as high mobility metallic behavior between two insulating oxide, superconductivity, interface ferroelectricity, unusual magnetism, multiferroicity etc. has been observed at oxide interface making it an interesting field of study. We have shown that variable energy photoemission spectroscopy with high photon energies, can be a useful tool to realize such interfaces and controlling the properties of multilayered devices, as well as to understand the origin of unusual phenomenon exists at several multilayer interfaces. Chapter1 provides a brief description of low dimensional materials, overall perspective of interesting properties in materials with reduced dimensionality. We have emphasized on the importance of determining the internal structure of buried interface of different dimensionalities. We have given a brief overview and importance of different interfaces that we have studied in the subsequent chapters dealing with specific interfaces. Chapter 2 describes experimental and theoretical methods used for the study of interface and self-assembly reported in this thesis. These methods are divided into two categories. The first section deals with different experimental techniques, like, UV-Visible absorption and photoluminescence spectroscopy, X-Photoelectron Spectroscopy(XPS), X-Ray diffraction, Transmission Electron Microscopy(TEM) etc. This section also includes brief overview on synchrotron radiation and methods used for detail analysis of interface structure using variable energy XPS. In the second part of this chapter, we have discussed theoretical methods used in the present study. \ In Chapter 3A we have combined low energy XPS, useful to extract information of the surface of the nanoparticles, with high energy XPS, important to extract bulk information and have characterized the internal structure of nanoparticle system of different heterogeneity. We have chosen two important heterostructure systems namely, inverted core-shell(CdScore-CdSeshell) type nanoparticles and homogeneous alloy(CdSeS)type nanoparticles. Such internal structure study revealed that the actual internal structure of certain nanomaterial can be widely different from the aim of the synthesis and knowledge of internal structure is a prerequisite in understanding their property. We were able to extend the idea of variable energy XPS to higher energy limit. Many speculations have been made about the probable role of interface in controlling properties, like blinking behavior of bigger sized core-shell nanoparticles, but no conclusive support has yet been given about the nature of such interface. After successfully extending the technique to determine the internal structure of heterostructured nanoparticles to very high photon energy region, we took the opportunity to determine the internal structure of nanoparticles of sizes as large as 12nm with high energy photoemission spectroscopy for the first time. In Chapter 3B we emphasize on the importance of interface structure in controlling the behavior of bigger sized nanoparticles systems, the unsettled issues regarding their internal structure, and described the usefulness of high energy XPS in elucidating the internal structure of such big particles with grate accuracy to solve such controversies. The existence of high density storage media relies on the existence of highly sensitive magnetic sensors with large magnetoresistance. Today almost all sensor technologies used in modern hard disk drives rely on tunnel magnetoresistance (TMR) CoFeB-MgO-CoFeB structures. Though device fabrication is refined to meet satisfactory quality assurance demands, fundamental understanding of the refinement in terms of its effect on the nature of the interfaces and the MgO tunnel barrier leading to improved TMR is still missing. Where, the annealing condition required to improve the TMR ratio is itself not confirmatory its effect on the interface structure is highly debatable. In particular, it has been anticipated that under the proposed exotic conditions highly mobile B will move into the MgO barrier and will form boron oxide. In Chapter 4 we are able to shed definite insights to heart of this problem. We have used high energy photoemission to investigate a series of TMR structures and able to provide a systematic understanding of the driving mechanisms of B diffusion in CoFeBTMR structures. We have solved the mix-up of annealing temperature required and have shown that boron diffusion is limited merely to a sub-nanometer thick layer at the interface and does not progress beyond this point under typical conditions required for device fabrication. We have given a brief overview on the evolution of magnetic storage device and have described various concepts relevant for the study of such systems. The interface between two nonmagnetic insulators LaAlO3 and SrTiO3 has shown a variety of interface phenomena in the recent times. In spite of a large number of high profile studies on the interface LaAlO3 and SrTiO3 there is still a raging debate on the nature, origin and the distribution of the two dimensional electron gas that is supposed to be responsible for its exotic physical properties, ranging from unusual transport properties to its diverse ground states, such as metallic, magnetic and superconducting ones, depending on the specific synthesis. The polar discontinuity present across the SrTiO3-LaAlO3 interface is expected to result in half an electron transfer from the top of the LaAlO 3 layer to each TiofSrTiO3 at the interface, but, the extent of localization that can make it behave like delocalized with very high mobility as well as localized with magnetic moments is not yet clear. In Chapter 5 we have given a description of this highly interesting system as well as presented the outcome of our depth resolved XPS investigation on several such samples synthesized under different oxygen pressure. We were able to describe successfully the distribution of charge carriers. While synthesizing and understanding properties of nanoparticles is one issue, using them for device fabrication is another. For example, to make a certain device often requires specific arrangements of nanoparticles in a suitable substrate. Self-assembly formation can be a potential tool in these regards. Just like atom or ions, both nano and colloidal particles also assemble by themselves in ordered or disordered structure under certain conditions, e.g., the drying of a drop of suspension containing the colloid particles over a TEM grid. This phenomenon is known as self-assembly. Though, the process of assembly formation can be a very easy and cost-effective technique to manipulate the properties in the nano region, than the existing ones like lithography but, the lack of systematic study and poor understanding of these phenomena at microscopic level has led to a situation that, there is no precise information available in literature to say about the nature of such assembly. In Chapter 6 we have described experiments that eliminate the dependence of the self-assembly process on many complicating factors like substrate-particle interaction, substrate-solvent interaction etc., making the process of ordering governed by minimum numbers of experimental parameter that can be easily controlled. Under simplified conditions, our experiments unveil an interesting competition between ordering and jamming in drying colloid systems similar to glass transition phenomenon Resulting in the typical phase behavior of the particles. We establish a re-entrant behavior in the order-disorder phase diagram as a function of particle density such that there is an optimal range of particle density to realize the long-range ordering. The results are explained with the help of simulations and phenomenological theory. In summary, we were able to extend the idea of variable energy XPS to higher energy limit advantageous for investigating internal structure of nonmaterial of various dimensionalities and sizes. We were able to comprehend nature of buried interface indicating properties of heterostructures quantum dots and thin films. Our study revealed that depth resolved XPS combined with accessibility of high and variable energies at synchrotron centers can be a very general and effective tool for understanding buried interface. Finally, we have given insight to the mechanism of spontaneous ordering of nanoparticles over a suitable substrate.