This thesis presents some theoretical studies dealing with quantum interference effects in electron transport through single molecule magnet transistors and a study on optical non-conserving spin transitions in the Nitrogen-vacancy center in diamond. The thesis starts with a brief general introduction to the physics of quantum transport through single electron transistors. Afterwards, the main body of the thesis is divided into three studies: (i) In chapter (2) we describe the properties of single molecule magnets and the Berry phase interference present in this nanomagnets. We then propose a way to detect quantum interference experimentally in the current of a single molecule magnet transistor using polarized leads. We apply our theoretical results to the newly synthesized nanomagnet Ni4. (ii) In chapter (3) we review the Kondo effect and present a microscopic derivation of the Kondo Hamiltonian suitable for full and half integer spin nanomagnets. We then calculate the conductance of the single molecule magnet transistor in the presence of the Kondo effect for Ni4 and show how the Berry phase interference becomes temperature dependent. (iii) We conclude in chapter (4) with a theoretical study of the single Nitrogen vacancy defect center in diamond. We show that it is possible to have spin non-conserving transitions via the hyperfine interaction and propose a way to write and read quantum information using circularly polarized light by means of optical Lambda transitions in this solid state system.

<p dir="ltr">A bath of free electrons interacting with a local quantum impurity leads to various exotic non-Fermi liquid behaviors, such as the non-integer effective ground state degeneracy of the impurity and the correction to the zero temperature conductance, which is temperature to the power of a fractional number. The former indicates emergent anyons, which are the key ingredients for achieving topological protected quantum computations. The latter can be used for experimentally probing non-Fermi liquid physics. It was recently proposed that a Coulomb blockaded M-Majorana island coupled to normal metal leads realizes a novel type of Kondo effect where the effective impurity “spin” transforms under the orthogonal group SO(M). Inspired by the multichannel generalization of the original Kondo model, we introduce a physically motivated N-channel generalization of this topological Kondo model whose impurity spin stems from the non-local topological ground state degeneracy of the island. This multichannel topological Kondo model supports Z3 parafermion and Fibonacci anyon (not supported by one-channel topological Kondo model) but may be limited to experiments because it is unstable to channel anisotropy. Therefore, we propose a Majorana-free meso- scopic setup which implements the Kondo effect of the symplectic Lie group and can harbor emergent anyons (including Majorana fermions, Fibonacci anyons, and Z3 parafermions) even in the absence of perfect channel symmetry. Besides, I comment on the future work such as the strong tunneling case that is beyond the topological Kondo regime and the two-impurity Kondo physics.</p>

Cette thèse en électronique moléculaire porte essentiellement sur le développement d’une méthode pour le calcul de la transmission de dispositifs électroniques moléculaires (DEMs), c’est-à-dire des molécules branchées à des contacts qui forment un dispositif électronique de taille moléculaire. D’une part, la méthode développée vise à apporter un point de vue différent de celui provenant des méthodes déjà existantes pour ce type de calculs. D’autre part, elle permet d’intégrer de manière rigoureuse des outils théoriques déjà développés dans le but d’augmenter la qualité des calculs. Les exemples simples présentés dans ce travail permettent de mettre en lumière certains phénomènes, tel que l’interférence destructive dans les dispositifs électroniques moléculaires. Les chapitres proviennent d’articles publiés dans la littérature. Au chapitre 2, nous étudions à l’aide d’un modèle fini avec la méthode de la théorie de la fonctionnelle de la densité de Kohn-Sham un point quantique moléculaire. De plus, nous calculons la conductance du point quantique moléculaire avec une implémentation de la formule de Landauer. Nous trouvons que la structure électronique et la conductance moléculaire dépendent fortement de la fonctionnelle d’échange et de corrélation employée. Au chapitre 3, nous discutons de l’effet de l’ajout d’une chaîne ramifiée à des molécules conductrices sur la probabilité de transmission de dispositifs électroniques moléculaires. Nous trouvons que des interférences destructives apparaissent aux valeurs propres de l’énergie des chaînes ramifiées isolées, si ces valeurs ne correspondent pas à des états localisés éloignés du conducteur moléculaire. Au chapitre 4, nous montrons que les dispositifs électroniques moléculaires contenant une molécule aromatique présentent généralement des courants circulaires qui sont associés aux phénomènes d’interférence destructive dans ces systèmes. Au chapitre 5, nous employons l’approche « source-sink potential » (SSP) pour étudier la transmission de dispositifs électroniques moléculaires. Au lieu de considérer les potentiels de sources et de drains exactement, nous utilisons la théorie des perturbations pour trouver une expression de la probabilité de transmission, T(E) = 1 − |r(E)|2, où r(E) est le coefficient de réflexion qui dépend de l’énergie. Cette expression dépend des propriétés de la molécule isolée, en effet nous montrons que c’est la densité orbitalaire sur les atomes de la molécule qui sont connectés aux contacts qui détermine principalement la transmission du dispositif à une énergie de l’électron incident donnée. Au chapitre 6, nous présentons une extension de l’approche SSP à un canal pour des dispositifs électroniques moléculaires à plusieurs canaux. La méthode à multiples canaux proposée repose sur une description des canaux propres des états conducteurs du dispositif électronique moléculaire (DEM) qui sont obtenus par un algorithme auto-cohérent. Finalement, nous utilisons le modèle développé afin d’étudier la transmission du 1-phényl-1,3-butadiène branché à deux rangées d’atomes couplées agissant comme contacts à gauche et à la droite. / This thesis is on molecular electronics concentrates mostly on the development of a method for the calculation of the transmission probability of molecules that are connected to contacts. On the one hand, this method aims at bringing a different point of view among the other methods for such calculations. On the other hand, it allows the integration of already developed theoretical tools in a rigorous manner, which increases the quality of the calculations. The work presented here often contains simple examples that shine some light on phenomena, such as the destructive interference, in molecular electronic devices. The chapters are from articles already published in the litterature. In chapter 2, we study a molecular quantum dot using a finite model with Kohn-Sham density functional theory. Moreover, using an implementation of the Landauer formula, we calculate the conductance of the quantum dot. We find that the electronic structure and molecular conductance depend strongly on the exchange and correlation functional employed. In chapter 3, we discuss the effect of adding a side chain to conducting molecules on the transmission probability of molecular electronic devices. We find that destructive interferences appear approximately at the energy eigenvalues of the isolated side chain, if these values do not correspond to localized states far away from the conductor. In chapter 4, we show that molecular electronic devices containing an aromatic molecule generaly possess circular currents which are associated with destructive interference phenomena in these systems. In chapter 5, we use the source-sink potential (SSP) approach to study the electronic transmission of some devices. Instead of considering the source and sink potentials exactly, we use perturbation theory to find an expression for the transmission probability T(E) = 1 − |r(E)|2 that depends on the properties of the bare molecule, where r(E) is the energy-dependent reflection coefficient. We show that in the first-order, it is the orbital density on the atoms connected to the contacts that largely determines the transmission probability for a given incoming electron energy. In chapter 6, we present an extension of the single channel source-sink potential approach for molecular electronic devices to multiple channels. The proposed multichannel method relies on an eigenchannel description of the conducting states of the molecular electronic device, which are obtained by a self-consistent algorithm. We use the model to study the transport of the 1-phenyl-1,3-butadiene molecule connected to two coupled rows of atoms that act as contacts on the left and right sides.

Aujourd'hui, nos appareils électroniques sont de plus en plus densément composés de composants nanoélectroniques. En conséquence, la dissipation de chaleur produite dans ces circuits augmente également énormément, provoquant une déperdition d’énergie considérable, en pure perte. Les effets thermoélectriques entrent en jeu ici car ils permettent d'utiliser cette chaleur perdue pour produire un travail utile. Par conséquent, l’étude du transport thermique et de l’effet thermoélectrique dans les nanostructures revêt une importance significative du point de vue scientifique et technologique.Dans cette thèse, nous présentons nos études expérimentales du transport thermique et thermoélectrique dans différents types de dispositifs à un seul électron, où le flux électronique peut être contrôlé au niveau de l'électron unique.Tout d’abord, nous montrons la mesure du transport de chaleur contrôlé par la grille dans un transistor à un seul électron (SET), agissant comme un commutateur thermique entre deux réservoirs. Nous déterminons la conductance thermique à l’aide d’un bilan thermique en régime permanent prenant en compte les différents chemins du flux de chaleur. La comparaison de la conductance thermique du SET avec sa conductance électrique indique une forte violation de la loi de Wiedemann-Franz.Deuxièmement, nous étendons l’étude du transport thermique dans les dispositifs à un seul électron dans le régime de boîte quantique, où, outre les interactions de Coulomb, il faut également prendre en compte les différents niveaux électroniques discrets. Nous discutons du bilan thermique entre deux réservoirs de chaleur couplés par un seul niveau de point quantique, et de la dissipation des électrons tunnel dans les contacts. Cela produit des formes de diamant de Coulomb dans la carte de température électronique de la source, en fonction de la polarisation et de la tension de grille.Enfin, nous présentons la mesure du transport thermoélectrique dans une jonction à boîte quantique unique, du régime de couplage faible au régime de couplage fort Kondo. Nos expériences introduisent une nouvelle façon de mesurer le pouvoir thermoélectrique en réalisant une condition de circuit ouvert quasi-parfaite. Le pouvoir thermoélectrique dans une boîte faiblement couplée montre le comportement e-périodique avec la charge induite par la grille, alors qu’il montre une période distincte de 2e en présence de corrélation Kondo. L’étude de la dépendance thermique révèle que la résonance de Kondo n’est pas toujours au niveau de Fermi, mais qu’elle peut être légèrement décalée, en accord avec les prédictions théoriques.Cette étude ouvre la porte à l’étude de transistors à une boîte quantique unique dont les propriétés thermodynamiques sont régies par les lois de thermodynamique quantique. / At this age of technologically advanced world, the electronic devices are getting more and more densely packed with micro-electronic elements of nano-scale dimension. As a result the heat dissipation produced in these microelectronic-circuits is also increasing immensely, causing a huge amount of energy loss without any use. The textit{thermoelectric effects} come into play here as one can use this wasted heat to produce some useful work with the help of thermoelectric conversion. In order to achieve such a textit{heat engine} with a reasonably high efficiency, one needs to understand its thermal behavior at the basic level. Therefore, the study of thermal transport and thermoelectric effect in nano-structures has significant importance both from scientific and application point of view.In this thesis we present the experimental studies of thermal and thermoelectric transport in different kinds of single-electron devices, where the electronic flow can be controlled at the single electron level.First, we demonstrate the measurement of gate-controlled heat transport in a Single-Electron Transistor ($SET$), acting as a heat switch between two heat reservoirs. The measurement of temperature of the leads of the $SET$ allows us to determine its thermal conductance with the help of a steady state heat-balance among all possible paths of heat flow. The comparison of thermal conductance of the $SET$ with its electrical conductance indicates a strong violation of the Wiedemann-Franz (WF) law away from the charge degeneracy.Second, we extend the study of thermal transport in single-electron devices to the quantum limit, where in addition to the Coulomb interactions the quantum effects are also need to be taken into account, and therefore the individual discrete electronic levels take part in the transport process. We discuss the heat-balance between two heat reservoirs, coupled through a single Quantum-Dot ($QD$) level, and the dissipation of the tunneling electrons on the leads. This produces Coulomb-diamond shapes in the electronic-temperature map of the `source' lead, as a function of bias and gate voltage.Third, we present the measurement of thermoelectric transport in a single $QD$ junction, starting from the weak coupling regime to the strong coupling-Kondo regime. The experiments introduces a new way of measuring thermovoltage realizing a close to perfect open-circuit condition. The thermopower in a weakly coupled $QD$ shows an expected `$e$' periodic behavior with the gate-induced charge, while it shows a distinct `$2e$' periodic feature in the presence of Kondo spin-correlation. The temperature dependence study of the Kondo-correlated thermopower reveals the fact that the Kondo-resonance is not always pinned to the Fermi level of the leads but it can be slightly off, in agreement with the theoretical predictions.This study opens the door for accessing a single $QD$ junction to operate it as a $QD$-heat engine, where the thermodynamic properties of the device are governed by the laws of textit{quantum thermodynamics}.

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We investigate the manifestation of strong electronic correlations in the quasiparticle interference (QPI), arising from the scattering of conduction electrons from defects and impurities in an otherwise translationally-invariant host. The QPI may be measured experimentally as the Fourier transform of the spatial modulations in the host surface density of states that result, which are mapped using a scanning tunnelling microscope. We calculate the QPI for a range of physically relevant models, demonstrating the effect of strong local electronic correlations arising in systems of magnetic impurities adsorbed on the surface of non-interacting host systems. In the first instance the effect of these magnetic impurities is modelled via the single Anderson impurity model, treated via numerical renormalization group (NRG) calculations. The scattering of conduction electrons, and hence the QPI, demonstrate an array of characteristic signatures of the many-body state formed by the impurity, for example due to the Kondo effect. The effect of multiple impurities on the QPI is also investigated, with a numerically-exact treatment of the system of two Anderson impurities via state-of-the-art NRG calculations. Inter-impurity interactions are found to result in additional scattering channels and additional features in the QPI. The QPI is then investigated for the layered transition metal oxide Sr2RuO4, for which strong interactions in the host conduction electrons give rise to an unconventional triplet superconducting state at T_c &Tilde; 1.5K. The detailed mechanism for this superconductivity is still unknown, but electron-electron or electron-phonon interactions are believed to play a central role. We simulate the QPI in Sr₂RuO₄, employing an effective parametrized model consisting of three conduction bands derived from the Ru 4d t2g orbitals that takes into account spin orbit coupling and the anisotropy of the Ru t2g orbitals. Signatures of such interactions in the normal state are investigated by comparing these model calculations to experimental results. We also calculate the QPI in the superconducting state, and propose how experimental measurements may provide direct evidence of the anisotropy and symmetry of the superconducting gap, and thus offer insight into the pairing mechanism and the superconducting state.

[pt] Esta tese investiga as propriedades eletrônicas de sistemas nanoscópicos com interações de muitos corpos, dando origem ao efeito Kondo. Primeiramente estudamos a transição SU(4)-SU(2) devido a um campo magnético externo e as propriedades de filtro de spin de um nanossistema de dois pontos quânticos capacitivamente acoplados. A transição é caracterizada pela diferença entre as polarizações de spin da ocupação eletrônica nos dois pontos quânticos, como uma função do potencial de porta aplicado sobre os pontos quânticos. Apesar do fato de que o campo magnético externo quebra a simetria SU(4) do Hamiltoniano, o estado fundamental a preserva, como uma propriedade emergente, na região do espaço de parâmetros onde os elétrons não estão polarizados. As propriedades de filtro de spin devido à população eletrônica spin polarizada nos pontos quânticos também é discutida. Estas propriedades são estudadas usando o formalismo dos operadores de projeção, que descreve de forma muito acurada a física associada ao estado fundamental dos sistemas Kondo. No capítulo subsequente, analisamos os efeitos da interação spin-órbita num ponto quântico conectado a contatos, representados pelo modelo da impureza de Anderson no efeito Kondo. Contrariamente ao resultado prévio de vários outros autores, nós mostramos que a interação spin-órbita reduz exponencialmente a temperatura Kondo enquanto a ação da interação no próprio ponto quântico pode ser um mecanismo de destruição do regime Kondo, conforme quebra a simetria SU(2). Usando o modelo de Anderson com acoplamento spin-órbita nós propomos um transistor de spin feito de um ponto quântico conectado a uma nanofaixa submetida à interação spin-órbita Rashba, depositada sobre um substrato ferromagnético. O ponto quântico também é conectado a dois contatos metálicos laterais, através do qual a corrente flui ao longo do sistema. A interação spin-órbita Rashba cria um mecanismo de inversão do spin no ponto quântico. Nós mostramos que o sistema é capaz de operar como um transistor de spin. / [en] This thesis investigates the electronic properties of nanoscopic systems under the presence of many body interactions, given rise to the Kondo effect. Firstly we studied the SU(4)-SU(2) crossover driven by an external magnetic field and the spin-filter properties of a capacitively coupled double quantum dot nanosystem. The crossover is characterized by the difference between the spin polarization of the electronic occupation at the double quantum dot, as a function of the gate potential applied to the quantum dots. Despite the fact that the external magnetic field breaks the SU(4) symmetry of the Hamiltonian, the ground state preserves it, as an emergent property, in a region in the parameter space where the electron are not polarized. The spinfilter properties due the spin polarized electronic population at the dots is also discussed. These properties are studied using the projector projection operator approach, which describes very accurately the physics associated to the ground state of Kondo systems. In a subsequent chapter, we analyze the effect of the spin-orbit interaction in a quantum dot connected to leads, represented by the Anderson impurity model on the Kondo effect. Contrary to several other authors previous results, we show that the Rashba spin-orbit interaction exponentially reduces the Kondo temperature while the action of the interaction on the quantum dot itself could be a mechanism of destroying the Kondo regime, as it breaks SU(2) symmetry. Using the Anderson model with spin-orbit coupling we propose a spin transistor device made of a quantum dot connected to a Rashba spinorbit interacting nanoribbon, deposited on a ferromagnetic substrate. The quantum dot is also connected to two lateral metallic contacts, through which the current flows along the system. The Rashba spin-orbit interaction creates a spin-flip mechanism at the quantum dot. We show that the system is capable of operating as a spin-transistor.

[pt] Nesta tese foram estudados três sistemas nanoscópicos compostos de pontos quânticos (PQs). No primeiro deles foi analisada a denominada nuvem Kondo, ou a extensão da blindagem que os spins da banda de condução fazem do spin de uma impureza magnética embebida em uma matriz metálica e representada, no nosso caso, por um PQ. As propriedades da nuvem Kondo foram obtidas através da manifestação da ressonância Kondo na densidade de estados local nos sítios da matriz metálica e também através das correlações de spin entre o spin do elétron no PQ e os spins da banda de condução. Foi possível encontrar uma concordância entre as extensões da nuvem Kondo obtidas com ambos métodos. O segundo sistema estudado consiste em uma estrutura de três PQs alinhados e com o PQ central acoplado a dois contatos metálicos. Foi analisada a operação deste sistema como uma porta lógica quântica cujo funcionamento depende do estado de carga do PQ central. Foi feito um estudo dependente do tempo das propriedades do sistema e, em particular, da correlação dos spins dos PQs laterais. Mostramos que o efeito Kondo, refletido na condutância do sistema, pode ser uma ferramenta fundamental para conhecer o estado da porta quântica. Os primeiros dois sistemas foram tratados usando o método dos Bósons Escravos na aproximação de campo médio. Finalmente, foi estudado o transporte termoelétrico em um sistema de dois PQs quando um deles está acoplado a contatos metálicos unidimensionais. O sistema foi analisado no regime de resposta linear e não linear a um potencial externo no regime de bloqueio de Coulomb. Mostramos que a presença de ressonâncias Fano e de uma singularidade de Van-Hove na densidade de estados dos contatos unidimensionais perto do nível de Fermi são ingredientes fundamentais para o aumento da eficiência termoelétrica do dispositivo. O problema de muitos corpos foi resolvido na aproximação de Hubbard III que permite um estudo correto das propriedades de transporte deste sistema para T maior que TK, onde TK é a temperatura Kondo. / [en] In this thesis, were studied three nanoscopic quantum dot (QD) systems. First, the so-called Kondo cloud was analyzed, the extension of the conduction band spin screening of a magnetic impurity embedded in a metallic matrix and represented, in our case, by a QD. The Kondo cloud properties were obtained studying the way in which the local density of states of the metallic matrix sites reflects the Kondo resonance and also through the spin-spin correlations between the QD and the conduction band spins. It was possible to find a good agreement between the Kondo cloud extensions obtained using both methods. The second system consists of three aligned QDs with the central QD connected to two metallic leads. The operation of this system as a quantum gate was studied, which depends on the central QD charge. A time dependent study of the system properties and, in particular, of the lateral QDs spin correlation was developed. We showed that the Kondo effect, reflected in the conductance, could be a fundamental tool to measure the information contained in the quantum gate state. The first two systems were treated using the Slave Bosons Mean Field Approximation method. Finally, we studied the thermoelectric transport of a two QD system when one of them is connected to two onedimensional leads. The system was analyzed in the linear and nonlinear response to an external applied potential, always in the Coulomb blockade regime. It was found that the presence of Fano resonances and a Van-Hove singularity in the one-dimensional lead density of states near the Fermi level are fundamental ingredients to enhance thermoelectric efficiency. The many-body problem was treated in the Hubbard III approximation, which is a correct approach to study the transport properties for T greater than TK, where TK is the Kondo temperature.

Les circuits électroniques mesurés à des températures cryogéniques permettent d'étudier le comportement quantique des électrons. En particulier, les circuits de boites quantiques sont des systèmes accordables modèles pour l'étude des électrons fortement corrélés, symbolisée par l'effet Kondo. Dans cette thèse, des circuits de boîtes quantiques à base de nanotube de carbone sont intégrés à des cavités micro-onde coplanaires, avec lesquelles l'électrodynamique quantique en cavité (cQED) a atteint un degré de contrôle remarquable de l'interaction lumière-matière. Les photons de la cavité micro-onde sont ici utilisés pour sonder la dynamique de charge dans le circuit de boîtes quantiques. Plus précisément, la cavité micro-onde de grande finesse nous a permis de mesurer la compressibilité du gas d'électrons dans une boîte avec une sensibilité sans précédent. Des mesures simultanées de transport électronique et de la compressibilité montrent que la résonance Kondo observées dans la conductance est transparente aux photons micro-ondes. Cela révèle le gel de la dynamique de charge dans la boîte quantique pour ce mécanisme particulier de transport d'électrons et illustre que la résonance Kondo à N-corps dans la conductance est associée aux corrélations issues des fluctuations de spin d'une charge gelée. Nous étudions aussi dans cette thèse la possible émergence d'une nouvelle quasi-particule, appelée état lié de Majorana, et qui serait sa propre anti-particule. Dans ce but, une grille ferromagnétique a été placée sous le nanotube pour créer un couplage spin-orbit artificiel. L'observation d'états d'Andreev dans un tel dispositif est un premier pas prometteur vers la détection avec une architecture cQED d'états liés de Majorana dans les nanotubes de carbone. / On-chip electronic circuits at cryogenic temperature are instrumental to studying the quantum behavior of electrons. In particular, quantum dot circuits represent tunable model systems for the study of strong electronic correlations, epitomized by the Kondo effect. In this thesis, carbon nanotube based-quantum dot circuits are embedded in coplanar microwave cavities, with which circuit quantum electrodynamics (cQED) has reached a high degree of control of the light-matter interaction. Here, microwave cavity photons are used to probe the charge dynamics in the quantum dot circuit. More precisely, the high finesse cavity allows us to measure the compressibility of the electron gas in the dot with an unprecedented sensitivity. Simultaneous measurements of electronic transport and compressibility show that the Kondo resonance observed in the conductance is transparent to microwave photons. This reveals the predicted frozen charge dynamics in the quantum dot for this peculiar electron transport mechanism and illustrates that the many-body Kondo resonance in the conductance is associated to correlations arising from spin fluctuations of a frozen charge. A second quantum phenomenon addressed in this thesis is the possible emergence of a new quasi-particle in condensed matter, called Majorana bound state, which would be its own anti-particle. For that purpose, a ferromagnetic gate has been placed below a nanotube in order to generate a synthetic spin-orbit coupling. The observation of Andreev bound states in such a device is a first promising step towards the detection with a cQED architecture of Majorana bound states in a carbon nanotube.