No description available.

Transition metal oxides (TMO) have proven to exhibit novel properties such as high temperature superconductivity, magnetic ordering, charge and spin density waves, metal to insulator transitions and colossal magnetoresistance. Among these are a spin-orbit coupling (SOC) induced Mott insulator Sr2IrO4. The electric transport properties of this material remain finite even at cryogenic temperatures enabling its complex electronic structure to be investigated by a scanning tunneling microscope. At T = 77 K, we observed two features which represent the Mott gap with a value of 2D ~ 615 meV. Additionally an inelastic loss feature was observed inside this gap due to a single magnon excitation at an energy of ~ 125 meV. These features are consistent with similar measurements with other probes. In addition to these features, at T = 4.2 K lower energy features appear which are believed to be due to additional magnetic ordering. Another material that exhibits a unique physical behavior is the sliding charge density wave (CDW) material TaS3. It is a quasi-one dimensional material that forms long narrow ribbon shaped crystals. It exhibits anomalies including non-ohmic conductivity, a decrease in the Young’s modulus, a decrease in the shear modulus and voltage induced changes in the crystal’s overall length. In addition, we have observed the torsional piezo-like response, voltage induced torsional strain (VITS), in TaS3 which was first discovered by Pokrovskii et. al. in 2007. Our measurements were conducted with a helical resonator. The VITS response has a huge effective piezoelectric coefficient of ~ 104 cm/V. In addition we have concluded that the VITS is a very slow response with time constants of ~ 1 s near the CDW depinning threshold, that these time constants are dependent on the CDW current, and we suggest that the VITS is due to residual twists being initially present in the crystal.

A microscopia de varredura por tunelamento (MVT) é uma nova maneira de se observar experimentalmente o efeito Kondo. Quando uma concentração de átomos é adicionada a um meio metálico (metal hospedeiro), a corrente de tunelamento passa a depender de fatores de origem não geométrica. O rearranjo das cargas dentro do volume metálico (oscilações de Friedel) e o espalhamento de spins eletrônicos (efeito Kondo), devido a introdução de impurezas, mudam o valor da corrente e influenciam o levantamento da topografia do espécime examinado. Esses fatores devem ser considerados para que a topografia gerada seja condizente com a topografia verdadeira. Utilizamos como modelo teórico para descrição desse sistema, o modelo de Anderson de uma impureza para simular o espécime examinado e uma banda de condução livre para representar os elétrons da agulha metálica do microscópio. Nossa abordagem usa a fórmula de Kubo para o cálculo da corrente de tunelamento, supondo Hamiltoniano de tunelamento como perturbação e o potencial elétrico no regime linear. Apresentamos inicialmente um estudo para o Modelo do Nível Ressonante, isto é, o modelo de Anderson sem correlação, com o objetivo de demonstrar a precisão do método do Grupo de Renormalização Numérico. Em seguida, analisamos o Modelo de Anderson correlacionado. Os resultados tanto para a condutância em função da distância entre ponta e impureza a temperatura fixa, como para condutância em função da temperatura e distância fixa, permitem interpretação física transparente desde que levem em conta a ressonância de Kondo na densidade espectral. / The scanning tunneling microscopy (STM) is a new way to observe experimentally the Kondo effect. When a concentration of atoms id added to a sample (host metal), the tunneling current begins to depend on other non-geometric factors. The rearrangement of charges in the metallic bulk (Friedel oscillations) and the electronic spin scattering (Kondo effect), due to the presence of impurities, change the current value and affect the sample´s topography. These factors must be considered in order to make a correspondence between the generated topography with the true one. As a theoretical description of the system, we use the single impurity Anderson model to simulate the examined sample and a free conduction band to represent the electrons of the microscope metallic tip. Our treatment uses the Kubo formula to calculate the tunneling current, assuming the tunneling Hamiltonian as a perturbation and the electric potential in the linear regime. We initially present a study of the Resonant Level Model, i.e, the Anderson model without correlaction, to show the accuary of the Numerical Renormalization Group procedure. In the next step, we analyse the correlated Anderson model. The dependence of the conductance on tip-impurity distance, at constant temperature, and its dependence on temperature for constant tip-impurity distance, allow a clear physical interpretation after taking into account the Kondo resonance in the spectral density.

A microscopia de varredura por tunelamento (MVT) é uma nova maneira de se observar experimentalmente o efeito Kondo. Quando uma concentração de átomos é adicionada a um meio metálico (metal hospedeiro), a corrente de tunelamento passa a depender de fatores de origem não geométrica. O rearranjo das cargas dentro do volume metálico (oscilações de Friedel) e o espalhamento de spins eletrônicos (efeito Kondo), devido a introdução de impurezas, mudam o valor da corrente e influenciam o levantamento da topografia do espécime examinado. Esses fatores devem ser considerados para que a topografia gerada seja condizente com a topografia verdadeira. Utilizamos como modelo teórico para descrição desse sistema, o modelo de Anderson de uma impureza para simular o espécime examinado e uma banda de condução livre para representar os elétrons da agulha metálica do microscópio. Nossa abordagem usa a fórmula de Kubo para o cálculo da corrente de tunelamento, supondo Hamiltoniano de tunelamento como perturbação e o potencial elétrico no regime linear. Apresentamos inicialmente um estudo para o Modelo do Nível Ressonante, isto é, o modelo de Anderson sem correlação, com o objetivo de demonstrar a precisão do método do Grupo de Renormalização Numérico. Em seguida, analisamos o Modelo de Anderson correlacionado. Os resultados tanto para a condutância em função da distância entre ponta e impureza a temperatura fixa, como para condutância em função da temperatura e distância fixa, permitem interpretação física transparente desde que levem em conta a ressonância de Kondo na densidade espectral. / The scanning tunneling microscopy (STM) is a new way to observe experimentally the Kondo effect. When a concentration of atoms id added to a sample (host metal), the tunneling current begins to depend on other non-geometric factors. The rearrangement of charges in the metallic bulk (Friedel oscillations) and the electronic spin scattering (Kondo effect), due to the presence of impurities, change the current value and affect the sample´s topography. These factors must be considered in order to make a correspondence between the generated topography with the true one. As a theoretical description of the system, we use the single impurity Anderson model to simulate the examined sample and a free conduction band to represent the electrons of the microscope metallic tip. Our treatment uses the Kubo formula to calculate the tunneling current, assuming the tunneling Hamiltonian as a perturbation and the electric potential in the linear regime. We initially present a study of the Resonant Level Model, i.e, the Anderson model without correlaction, to show the accuary of the Numerical Renormalization Group procedure. In the next step, we analyse the correlated Anderson model. The dependence of the conductance on tip-impurity distance, at constant temperature, and its dependence on temperature for constant tip-impurity distance, allow a clear physical interpretation after taking into account the Kondo resonance in the spectral density.

No description available.

Molecules adsorbed on two-dimensional (2D) materials can show interesting physical and chemical properties. This thesis presents scanning probe microscopy (SPM) investigation of emerging 2D materials, molecular nanostructures on 2D substrates at the nanometer scale, and biophysical processes on the biological membrane. Two main techniques of nano-probing are used: scanning tunneling microscopy (STM) and atomic force microscopy (AFM). The study particularly emphasizes on self-assembled molecules on flat 2D materials and quasi-1D wrinkles. First, we report the preparation of novel 1D C60 nanostructures on rippled graphene. Through careful control of the subtle balance between the linear periodic potential of rippled graphene and the C60 surface mobility, we demonstrate that C60 molecules can be arranged into a 1D C60 chain structure of two to three molecules in width. At a higher annealing temperature, the 1D chain structure transitions to a more closely packed, quasi-1D hexagonal stripe structure. The experimental realization of 1D C60 structures on graphene is, to our knowledge, the first in the field. It could pave the way for fabricating new C60/graphene hybrid structures for future applications in electronics, spintronic and quantum information. Second, we report a study on nano-morphology of potential operative donors (e.g., C60) and acceptors (e.g., perylenetetracarboxylic dianhydride, aka. PTCDA) on wrinkled graphene supported by copper foils. We realize sub-monolayer C60 and PTCDA on quasi-1D and quasi-2D real periodic wrinkled graphene, by carefully controlling the deposition parameters of both molecules. Our successful realization of acceptor-donor binary nanostructures on wrinkled graphene could have important implications in future development of organic solar cells. Third, we report an STM and spectroscopy study on atomically thin transition-metal dichalcogenides (TMDCs) material. TMDCs are emerging 2D materials recently due to their intriguing physical properties and potential applications. In particular, our study focuses on molybdenum disulfide (MoS2) mono- to few-layers and pyramid nanostructures synthesized through chemical vapor deposition. On the few-layered MoS2 nanoplatelets grown on gallium nitride (GaN) and pyramid nanostructures on highly oriented pyrolytic graphite (HOPG), we observe an intriguing curved region near the edge terminals. The measured band gap in these curved regions is consistent with the direct band gap in MoS2 monolayers. The curved features near the edge terminals and the associated electronic properties may contribute to understanding catalytic behaviors of MoS2 nanostructures and have potential applications in future electronic devices and catalysts based on MoS2 nanostructures. Finally, we report a liquid-cell AFM study on the endosomal protein sorting process on the biological lipid membrane. The sorting mechanism relies on complex forming between Tom1 and the cargo sorting protein, Toll interacting protein (Tollip). The induced conformational change in Tollip triggers its dissociation from the lipid membrane and commitment to cargo trafficking. This collaborative study aims at characterizing the dynamic interaction between Tollip and the lipid membrane. To study this process we develop the liquid mode of AFM. We successfully demonstrate that Tollip is localized to the lipid membrane via association with PtdIns3P (PI(3)P), a major phospholipid in the cell membrane involved in protein trafficking. / Ph. D.

Nous présentons un travail expérimental contribuant à l'étude de contacts ponctuels métalliques et moléculaires à l'aide de dispositifs de jonctions brisées développés dans notre équipe. Ces techniques de jonctions brisées, utilisables dans les conditions ambiantes, sont particulièrement adaptées à deux champs disciplinaires : l'électronique moléculaire et la nano mécanique.Nous avons étudié la durée de vie de contacts métalliques d'or, qui excède rarement la dizaine de millisecondes à température ambiante. Par le biais d'une analyse statistique de mesures de conductance, nous montrons que leur durée de vie est limitée par la contrainte mécanique appliquée à la jonction. Ces résultats nous ont permis de proposer un mécanisme de rupture, et de définir des conditions optimales pour la formation des contacts à température ambiante.Nous présentons ensuite une étude préliminaire de mesure de conductance d'une molécule unique, utilisant un dispositif à jonction brisée ainsi qu'un microscope à effet tunnel.Les résultats obtenus indiquent que, si la mesure de la conductance d'une molécule unique est possible, la stabilité observée est à considérer avant d'envisager des applications. / We present here an experimental work which contributes to the study of metallic and molecular point contacts using broken junctions-based devices developed in our team. Under ambient environmental conditions, these techniques are particularly adapted to two disciplinary fields: molecular electronics and nano-mechanics.We have studied the lifetime of gold contacts, which rarely exceed ten milliseconds at room temperature.Through statistical analyses of conductance measurements, we show that this lifetime is limited by the mechanical strain applied to the junction. These results allowed us to propose a breaking mechanism, and to define optimal conditions for the formation of the contacts at room temperature. We present then a preliminary study of conductance measurements of a single molecule, using a broken junction device as well as a scanning tunneling microscope.The results indicate that, despite the conductance measure of a single molecule is possible the observed stability should be considered before envisaging applications.

Technology where a solitary dopant acts as the active component of an opto-electronic device is an emerging  field known as solotronics, and bears the promise to revolutionize the way in which information is stored, processed and transmitted. Magnetic doped semiconductors and in particular (Ga, Mn)As, the archetype of dilute magnetic semiconductors, and topological insulators (TIs), a new phase of quantum matter with unconventional characteristics, are two classes of quantum materials that have the potential to advance spin-electronics technology. The quest to understand and control, at the atomic level, how a few magnetic atoms precisely positioned in a complex environment respond to external stimuli, is the red thread that connects these two quantum materials in the research presented here. The goal of the thesis is in part to elucidate the properties of transition metal (TM) impurities near the surface of GaAs semiconductors with focus on their response to local magnetic and electric fields, as well as to investigate the real-time dynamics of their localized spins. Our theoretical analysis, based on density functional theory (DFT) and using tight-binding (TB) models, addresses the mid-gap electronic structure, the local density of states (LDOS) and the magnetic anisotropy energy of individual Mn and Fe impurities near the (110) surface of GaAs. We investigate the effect of a magnetic field on the Mn acceptor LDOS measured in cross-sectional scanning tunneling microscopy, and provide an explanation of why the experimental LDOS images depend weakly on the field direction despite the strongly anisotropic nature of the Mn acceptor wavefunction. We also investigate the effects of a local electrostatic field generated by nearby charged As vacancies, on individual and pairs of ferromagnetically coupled magnetic dopants near the surface of GaAs, providing a means to control electrically the exchange interaction of Mn pairs. Finally, using the mixed quantum-classical scheme for spin dynamics, we calculate explicitly the time evolution of the Mn spin and its bound acceptor, and analyze the dynamic interaction between pairs of ferromagnetically coupled magnetic impurities in a nanoscaled semiconductor. The second part of the thesis deals with the theoretical investigation of a single substitutional Mn impurity and its associated acceptor state on the (111) surface of Bi2Se3 TI, using an approach that combines DFT and TB calculations. Our analysis clarifies the crucial role played by the spatial overlap and the quasi-resonant coupling between the Mn-acceptor and the topological surface states inside the Bi2Se3 band gap, in the opening of a gap at the Dirac point. Strong electronic correlations are also found to contribute significantly to the mechanism leading to the gap, since they control the hybridization between the p orbitals of nearest-neighbor Se atoms and the acceptor spin-polarization. Our results explain the effects of inversion-symmetry and time-reversal symmetry breaking on the electronic states in the vicinity of the Dirac point, and contribute to clarifying the origin of surface-ferromagnetism in TIs. The promising potential of magnetic-doped TIs accentuates the importance of our contribution to the understanding of the interplay between magnetic order and topological protected surface states.

Les dernières années ont vu l'avènement des couches cristallines bidimensionnelles, appelées matériaux 2D. L'exemple le plus connu est le graphène, d'autres étant le nitrure de bore hexagonal isolant et le diséléniure de niobium supraconducteur. Ces matériaux 2D peuvent être empilés de manière contrôlée sous la forme d'hétérostructures de van der Waals pour obtenir les propriétés électroniques désirées. L’une des plus simples hétérostructures de van der Waals est l'empilement de deux couches de graphène tournées. Cet empilement donne naissance à un moiré qui peut être vu comme un potentiel superpériodique dépendant de l'angle entre les deux couches. Les propriétés électroniques des couches tournées de graphène sont intimement liées à ce moiré.Le sujet de cette thèse est l'étude expérimentale du lien entre la structure et les propriétés électroniques des couches tournées de graphène par Microscopie et Spectroscopie à effet tunnel à basse température.Alors que l'effet de l'angle entre les couches sur les propriétés électroniques a déjà été étudié en détail, la modification de celles-ci par une déformation des couches n'a été envisagée que récemment. La première partie de ce travail expérimental étudie la modification par la déformation des propriétés électroniques de couches de graphène tournées d'un angle de 1.26° crûes sur carbure de silicium. La déformation en question est différente dans les deux couches et son effet apparait clairement dans la densité locale d'états électroniques du moiré. Contrairement à une déformation appliquée identiquement aux deux couches, une différence de déformations entre les couches (déformation relative) modifie fortement la structure de bandes même à faibles valeurs de déformations. Alors que la déformation relative était spontanément présente, la deuxième partie de cette thèse s'intéresse à l'effet d'une déformation appliquée directement aux couches de graphène. Cette déformation vient d'une interaction induite par l'approche de la pointe STM vers la surface de graphène. La modification active de la densité d'états qui en résulte dépend de la position de la pointe dans le moiré avec l'apparition d'instabilités périodiques lorsque la distance entre la pointe et l'échantillon est très faible.La troisième partie de cette thèse concerne l'étude d'un autre type de modification des propriétés électroniques consistant en l'induction de supraconductivité dans les couches de graphène. Cette modification est effectuée par une croissance du graphène en une seule étape sur du carbure de tantale supraconducteur. Les résultats montrent la formation d'une couche de carbure de tantale de grande qualité sur laquelle les couches de graphène forment des moirés. La mesure à basse température de la densité d'états de ces moirés montre la présence d'un effet de proximité supraconducteur induit par le carbure de tantale. / Recent years have seen the emergence of two-dimensional crystalline layers, called 2D materials. Examples include the well-known graphene, insulating hexagonal boron nitride and superconducting niobium diselenide. The stacking of these 2D materials can be controlled to achieve desirable electronic properties under the form of van der Waals heterostructures. One of the simplest van der Waals heterostructures is the misaligned stacking of two graphene layers. Twisted graphene layers show a moiré pattern which can be viewed as a superperiodic potential that depends on the twist angle. The electronic properties of the twisted graphene layers are strongly linked to this moiré pattern.The subject of the present thesis is the experimental study of the link between the structural and the electronic properties of twisted graphene layers by means of low-temperature Scanning Tunneling Microscopy and Spectroscopy (STM/STS).While the effect of the twist angle has already been studied in great details, the modulation of the electronic properties by the deformation of the layers has been explored only recently. In the first part of this experimental work, a strain-driven modification of the electronic properties is probed in graphene layers with a twist angle of 1.26° grown on silicon carbide. The determined strain is found to be different in the two layers leading to a clear signature in the local electronic density of states of the moiré even at low strain magnitudes. Contrary to a strain applied in the two layers, this difference of strain between the layers (relative strain) modifies strongly the electronic band structure even at low strain magnitudes. While this relative strain is natively present, the second part of the work explores the effect of an applied strain in the layers. This is realized by approaching the STM tip to the graphene surface to trigger an interaction between the two. The resulting active modification of the density of states is shown to depend on the position on the moiré, leading to periodic instabilities at very low tip-sample distances.In the third part of the work, another type of modification of the electronic properties is studied when superconductivity was induced in the graphene layers. This is done by growing graphene on superconducting tantalum carbide in a single-step annealing. The results show the formation of a high-quality tantalum carbide layer on which graphene layers form moiré patterns. The low-temperature density of states of these moirés show evidence of a superconducting proximity effect induced by the tantalum carbide.

No description available.