La dynamique des parois de domaine magnétiques (DW) soulève actuellement un très fort intérêt à la fois du point de vue fondamental mais aussi en lien avec ses applications dans des dispositifs logique et mémoire. Des dispositifs nouveaux basés sur les DW ont déjà été proposés, par exemple présentant des très fortes densités de stockage et des taux de transfert élevés pour un remplacement des disques durs. De plus dans les Mémoires Magnétiques à Accès Aléatoire (MRAM), identifiées comme l'une des solutions les plus prometteuses pour le remplacement des DRAM et SRAM, le retournement de l'aimantation implique une propagation des DW. Le contrôle de la dynamique des DW sous courant est longtemps resté un challenge, principalement à cause d'imperfections dans les matériaux utilisés. Des déplacements rapides et contrôlé des DW au moyen d'un courant ont été reportés il y a quelques années seulement dans des multicouches présentant une asymétrie d'inversion (SIA). Plus récemment un mécanisme a été proposé basé sur la présence de couple de spin orbite (SOT) et de l'interaction Dzyaloshinskii-Moriya (DMI), tout deux trouvant leur origine dans l'interaction spin-orbite et nécessitant une SIA.Mon objectif initial était de tester ce modèle dans deux systèmes présentant différents SIA. Dans des multicouches Pt/Co/Pt à faible SIA, j'ai étudié la propagation des DW sous courant et sous champ et j'ai mis en évidence l'existence d'un amortissement chiral. Ce phénomène nouveau, pendant de DMI pour les mécanismes dissipatifs, influence à la fois la dynamique sous courant et sous champ et doit être pris en compte pour avoir une description complète des mécanismes. Dans des multicouches Pt/Co/AlOx à fort SIA, j'ai étudié de nouvelles géométries pour lesquelles le mouvement de la paroi de domaine et la direction du courant ne sont pas colinéaires. J'ai mis en évidence un déplacement asymétrique des DW en fonction de cette non-colinéarité qui ne peut pas être expliquée avec un modèle simple DMI+SOT. En se basant sur ces résultats expérimentaux, j'ai introduit un nouveau concept de dispositifs, appelé « origami magnétique » : la forme du dispositif gouverne le mécanisme de retournement. Ce concept apporte une grande flexibilité dans la construction de mémoires magnétiques non volatiles, rapides et peu gourmandes en énergie : des fonctionnalités différentes peuvent être obtenues sur un même wafer simplement par la maîtrise de la forme des différents éléments. Je montre la preuve de concept de deux dispositifs. / Magnetic domain wall (DW) dynamics is currently attracting tremendous interest both from a fundamental point of view as well as in relation with emerging magnetic memory and logic devices. New DW-based devices were recently proposed, for example to replace hard drive disks with higher density and faster date transfer. Moreover, in Magnetic Random Access Memory (MRAM), identified as one of the most promising candidate for DRAM and SRAM replacement, switching occurs through DW propagation. Control of current induced DW dynamics has long been a challenge mainly due to material imperfections. Only some years ago, fast and controllable motions were reported in multilayers presenting structural inversion asymmetry (SIA). More recently, a mechanism was proposed based on the presence of spin orbit torques and Dzyaloshinskii-Moriya interaction (DMI), both phenomena originating from the spin orbit interaction and needing (SIA).My initial objective was to test this model in two systems presenting different SIA. In Pt/Co/Pt multilayers with weak SIA, I studied both current and field induced DW motion and evidenced a chiral damping. This new phenomena, counterpart of the DMI for the dissipative aspects, influences both current and field induced dynamics and has to be taken into account for a complete picture of the mechanism. In Pt/Co/AlOx multilayers with strong SIA, I studied new geometries where the DW motion the and current flow are not collinear. I evidenced asymmetric DW motion as a function of this non-collinearity that cannot be explained with a simple SOT+DMI model. Based on these experimental results I introduce a new device concept named “magnetic origami”: the shape of the device governs the switching mechanism. This concept provides large flexibility to construct fast, low power non-volatile magnetic memory: different functionalities can be achieved on a wafer by simply mastering the shape of the different elements. I show the proof of concept of two such devices.

[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.

La loi de Moore est basée sur l’observation empirique qu’environ chaque deux années, le nombre de transistors dans des circuits denses intégrées double. Cette tendance s'est bien maintenue au cours des dernières décennies (années 1970 et suivantes). Cependant, la miniaturisation continue des transistors entraîne une augmentation significative des pertes d’énergie par le courant de fuite, ce qui augmente la consommation d'énergie de veille. Cette perte d’énergie est devenue un problème majeur dans la microélectronique pendant les dernières années, ce qui rend plus difficile le développement des nouvelles technologies. L’une des solutions est de placer des éléments mémoire non-volatile dans le puce, qui retiennent la configuration du transistor pendant la mise hors tension et permettent de le restaurer à la mise sous tension. Les Magnetic Random Access Memories (MRAM) sont considérées par l'ITRS comme un candidat crédible pour le remplacement potentiel de SRAM et de DRAM au-delà du nœud technologique de 20 nm. Bien que les exigences de base pour la lecture et l'écriture d'un élément de mémoire unique sont remplies, l'approche actuelle basée sur Spin Torque Transfer (STT) souffre d'un manque inné de la flexibilité. Le courant électrique entraine le retournement de l’aimantation de la couche ferromagnétique libre par le transfert du moment angulaire d’une couche ferromagnétique adjacent. Ainsi les éléments de mémoire basées sur STT ont deux terminaux dont les voies de courant pour « écriture » et « lecture » sont définies par la forme de «pillar». L’optimisation indépendant des paramètres d’écriture et de lecture reste, donc, très difficile. Au même temps, la densité de courant trop haute, nécessaire pour écrire, conduit à la vieillissement prémature du jonction tunnel. En conséquence, l’intégration MRAM dans la technologie du semi-conducteur reste, donc, difficile.Démonstrations récentes de reversement d’aimantation entrainées par l’injection d’un courant planaire dans des heterostructures métal lourd/ferromagnet ont attiré l’attention croissante sur les couples de spin basé sur le transfert du moment angulaire par l’effet Hall de spin et les effets d’interface. Contrairement à STT-MRAM, la SOT-MRAM a trois terminaux, dont les voies de courant pour « écriture » et « lecture » sont indépendantes. Cela permet d’améliorer les paramètres « écriture » et « lecture » de manière indépendante. Pour contrôler et optimiser les SOT il est nécessaire de comprendre très bien leur origine. Cela reste l’une des plus importantes questions dont on n’a pas une réponse définitive. Dans ce contexte, plusieurs études ont conclu sur un modèle basé seulement sur l’effet Hall de spin, en même temps que d’autres ont suggéré un modèle basé sur une contribution combiné de l’effet Hall de spin et l’effet d’interface.L’objectif de cette thèse est de réaliser une étude systématique sur les effets d’interface sur les SOT dans des heterostructures métal lourde/ferromagnet a base de Pt, avec aimantation planaire.Dans ce but, cette thèse explore trois voies différentes. Premièrement nous avons modifié le rapport entre les effets d’interface et les effets bulk en changeant l’épaisseur de la couche de Pt et en suivant l’évolution des SOT. En deuxième nous avons exploré des différents empilements métal lourde/ferromagnet afin d’étudier différentes interfaces. Finalement, nous avons changé les propriétés des interfaces soit par changer la structure cristalline soit par oxydation. La technique de mesure, la méthode d’analyse de données associé et les aspects théoriques nécessaires pour l’interprétation des données sont aussi détaillés dans ce manuscrit. / Moore’s law is based on empirical observation and states that every two years approximately, the number of transistors in dense integrated circuits doubles. This trend has held up well in the past several decades (1970s and onwards). However, the continuous miniaturisation of transistors brings about a significant increase in leakage current, which increases the stand-by power consumption. This energy loss has become a major problem in microelectronics during the last several years, making the development of new technologies more difficult. One of the solutions that can address this issue is to place non-volatile memory elements inside the chip, that retain the configuration of the transistor during power-off and allow to restore it at power-on. Magnetic Random Access Memories (MRAM) are considered by the ITRS as a credible candidate for the potential replacement for SRAM and DRAM beyond the 20 nm technological node. Though the basic requirements for reading and writing a single memory element are fulfilled, the present approach based on Spin Transfer Torque (STT) suffers from an innate lack of flexibility. The electric current drives the magnetization switching of a free ferromagnetic layer by transferring angular momentum from an adjacent ferromagnet. Therefore, STT-based memory elements are two terminal devices in which the “pillar” shape defines both the “read” and the “write” current paths. Independent optimisation of the reading and writing parameters is therefore difficult, while the large writing current density injected through the tunnel barrier causes its accelerated ageing, particularly for fast switching. Consequently, the integration of MRAM into semiconductor technology poses significant difficulties.Recent demonstrations of magnetization switching induced by in-plane current injection in heavy metal (HM)/ferromagnet (FM) heterostructures have drawn increasing attention to spin-torques based on orbital-to-spin momentum transfer induced by Spin Hall and interfacial effects (SOTs). Unlike STT-MRAM, the in-plane current injection geometry of SOT-MRAM allows for a three-terminal device which decouples the “read” and “write” mechanisms, allowing the independent tuning of reading and writing parameters. However, an essential first step in order to control and optimise the SOTs for any kind of application, is to better understand their origin. The origin of the SOTs remains one of the most important unanswered questions to date. While some experimental studies suggest a SHE (Spin Hall Effect)-only model for the SOTs, others point towards a combined contribution of the bulk (SHE) and interface (Rashba Effect and Interfacial SHE). At the same time, many studies start with a SHE only hypothesis and do not consider interfacial effects. Furthermore, there are not so many systematic studies on the effects of interfaces. This thesis tries to fill in this gap, by providing a systematic study on the effects of interfaces on the SOTs, in Pt-based NM/FM/HM multilayers with in-plane magnetic anisotropy. For this purpose, this thesis explores three different, but related avenues. First, we changed the interface/bulk effect ratio by modifying the Pt thickness and following the evolution of the SOTs. Second, we explored different HM/FM/NM combinations, in order to study different interfaces. And third, we changed the properties of the interfaces by changing the crystallographic structure of the interface and by oxidation. The measurement technique and associated data analysis method, as well as the theoretical considerations needed for the interpretation of the results are also detailed in this manuscript.

Ce travail consiste en l'étude de phénomènes optomécaniques en d'interaction spin-orbite de la lumière, en utilisant des milieux inhomogènes et anisotropes comme systèmes modèles, différents types de systèmes matériels étant considérés en pratique. En particulier,nous avons utilisé des défauts de cristaux liquides nématiques pour lesquels nous avons identifié expérimentalement d'un couple optique de nature spin-orbite conduisant à des modifications de champ d'orientation moléculaire du cristal liquide. Aussi, grâce à l'utilisation de verres nanostructurés artificiellement permettant un contrôle de l'interaction spin-orbite à la demande,nous mettons en évidence un phénomène de couple optique inverse qui est l'analogue angulaire des forces optiques dites négatives. Cet effet optomécanique contre-intuitif est démontré expérimentalement, d'une manière indirecte, grâce à la mise en place de diverses expériences de décalage en fréquence Doppler associées aux degrés de liberté de rotation. Enfin, nous présentons nos tentatives en vue de réaliser expérimentalement l'observation directe d'un couple optique inverse. Plusieurs options sont envisagées, qui comprennent à la fois des approches à base de matériaux métalliques ou diélectriques. De manière générale, cela implique la miniaturisation des systèmes considérés, ce qui est effectué à la fois à l'échelle millimétrique et micrométrique. / This work focuses on angular optomechanics driven by the spin-orbit interaction of light, using inhomogeneous and anisotropic media as model systems and different kinds of such material systems are considered in practice. In particular, we use nematic liquid crystal defects and report on the direct experimental observation of spin-orbit optical radiation torque that leads to distortion of molecular orientation pattern of the defects. Then, by using solid-state spin-orbit couplers of arbitrary order made of artificially nanostructured glasses, we unveil an optical torque reversal phenomenon that is the angular counterpart of so-called optical negative forces. This counterintuitive optomechanical effect is experimentally retrieved, in an indirect manner, via rotational Doppler frequency shift experiments. Finally, we report on our attempts to build up an experimental framework allowing the direct observation of optical torque reversal. Several options are considered, which include both metallic and dielectric approaches and involve sample miniaturization that has been explored at the millimeter and micrometer scale.

Em sistemas com acoplamento spin-órbita (SO) é possível manipular eletricamente o spin do elétron via a aplicação de um campo elétrico.1 Isso permite a potencial aplicação do grau de liberdade de spin (Spintronica) no desenvolvimento de novos dispositivos e tecnologias, como por exemplo na tecnologia da informação (computação quântica).2,3 No entanto, sabe-se que a interação SO causa efeitos indesejáveis, como por exemplo a relaxação e o defasamento de spin.4 Dessa maneira, do ponto de vista de aplicações, torna-se desejável maximizar o tempo de vida do spin. Neste trabalho, investigamos a relaxação de spin dos elétrons de condução em poços quânticos com duas sub-bandas5 crescidos ao longo das direções [001] e [110] via o mecanismo de D\'yakonov-Perel\'.6 Combinando teoria de grupos, o método k.p, a aproximação da função envelope e teoria de perturbação de Löwdin obtemos um Hamiltoniano efetivo para os elétrons da banda de condução na presença das interações SO de Rashba e Dresselhaus. Aqui, diferentemente de alguns trabalhos anteriores,7,8 além de incluir o termo cúbico de Dresselhaus, também levamos em conta as contribuições devido à influência da segunda sub-banda de mais baixa energia do poço. A partir deste Hamiltoniano derivamos expressões para os tempos de relaxação do spin e analisamos como estas novas contribuições (termos do acoplamento com a segunda sub-banda) afetam os tempos de vida dos spins. Comparamos os tempos de relaxação para as direções [001] com os calculados para a direção [110]. Nossos resultados mostram que as contribuições devido à segunda sub-banda são desprezíveis para ambas as direções. Mostramos também que o tempo de relaxação para a direção [110] é mais longo que o da [001], resultado consistente com experimentos9,10 e outros trabalhos teóricos anteriores.7 / In systems with spin-orbit (SO) coupling, it is possible to electrically manipulate the electron spin via applied gate voltages.1 This allows for the potential use of the spin degree of freedom (Spintronics) in the development of new devices and technologies, for instance information technology (quantum computing).2,3 It is known however, that the SO interaction leads to the undesired effect of causing spin relaxation and spin dephasing.4 Thus from the point of view of applications, it is desirable to maximize the spin lifetimes. Here, we investigate the spin relaxation of the conduction electrons in quantum wells with two sub-bands5 grown along the [001] and [110] directions via the D\'yakonov-Perel\' mechanism.6 By combining group theory, the k.p method, the envelope function approach and the Löwdin perturbation theory, we obtain an effective Hamiltonian for the conduction electrons in the presence of the Rashba and Dresselhaus SO interactions. Differently from some early works,7,8 in addition to the cubic Dresselhaus term, we also account for the contributions arising from the second lowest sub-band of the well. We derive expressions for the spin relaxation times and analyze how the new contributions (second sub-band terms) affect the spin lifetimes. We compare the relaxation times obtained in the [001] direction with those calculated for the [110] direction. Our results show that the contributions from the second sub-band are negligible for both directions. We also find that the relaxation time in the [110] direction is longer than the one in the [001], a result consistent with experiments9,10 and earlier theoretical works.7

Made available in DSpace on 2016-06-02T20:15:31Z (GMT). No. of bitstreams: 1 5844.pdf: 11430873 bytes, checksum: b80a5790a9ebf6ae63ff48e52968ae60 (MD5) Previous issue date: 2014-02-21 / Universidade Federal de Sao Carlos / O crescimento e caracterização de sistemas de heteroestruturas semicondutoras quasi-unidimensionais têm atraído grande interesse devido à sua potencial de aplicação tecnológica, como foto-detectores, dispositivos opto-eletrônicos assim como seu para o processamento de informação quântica e aplicações em fotônica. O objetivo desta tese é o estudo das propriedades de transporte eletrônico e de spin em sistemas semicondutores quasi-unidimensionais, especificamente trataremos de nanofios (NWs) homogêneos, NWs acoplados, NWs do tipo plano-geminado (TP), diodos de tunelamento ressonante (ETD) e cadeias de pontos quânticos (QDCS). Escolhemos o método k-p, particularmente o Hamiltoniano de Luttinger, para descrever os efeitos de confinamento e tensão biaxial. Este sugeriu uma modulação do caráter do estado fundamental que, complementada com a dinâmica fônons fornecidas pelas simulações da Dinâmica Molecular (MD), permitiu a descrição da modulação da mobilidade de buracos por emissão ou absorção de fônons. Em relação ao sistema de NWs acoplado,estudamos, através do método da matriz de transferência (TMM), as propriedades de transporte de elétrons e spin sob a interação de spin-órbita (SOI) de Eashba, localizada na região de acoplamento entre fios. Foram consideradas várias configurações de tensões de gate (Vg) aplicadas nos fios. Desse modo, compreendemos a modulação do transporte de spin quando esse é projetado no direção-z através da combinação do SOI e das dimensionalidades do sistema. Da mesma forma, a combinação de SOI e da Vg aplicada deu origem a modulação da polarização, quando o spin medido é projetado na mesma direção em que o SOI de Eashba atua, a direção y. Usando o TMM, exploramos as propriedades de transporte de um DBS e o efeito de uma resistência em série com o intuito de provar a natureza da biestabilidade das curvas características I V bem como o aumento de sua área com temperatura, resultados fornecidos por experimentos. O modelo indicou que aumentando da resistência pela diminuição sa temperatura aumenta a área biestável. A presença de uma hetero-junção adicional ao sistema induz uma densidade de carga nas suas interfaces. De acordo com esta configuração, a queda de tensão total do ETDS muda, podendo ser confirmada experimentalmente. A formação dos peculiares campos de deformação e sua influência sobre a estrutura eletrônicas e propriedades de transporte em superredes de TP foi estudada sistematicamente. Assim, as propriedades de transporte, de ambos os elétrons e buracos, pode ser sintonizada eficientemente, mesmo no caso de elétrons r em sistemas de blenda de zinco, contrastando com a prevista transparência de elétrons r em superredes de semicondutores III-V heteroestruturados. Além disso, constatamos que a probabilidade de transmissão para buracos da banda de valência também poderia ser efetivamente modificada através de uma tensão externa.Por fim, colaboradores sintetizaram com sucesso sistemas de QDCs de InGaAs através da epitaxia de feixe molecular e engenharia de tensão. Um comportamento anisotrópico da condutância com a temperatura foi observado em QDCs com diferentes concentrações de dopagem, medida realizada ao longo e entre os QDCs. O modelo teórico 1D de hoppíng desenvolvido mostrou que a presença de estados OD modela a resposta anisotrópica da condutância neste sistemas. / The growth and characterization of semiconductor quasi-one-dimensional heterostructure systems have attracted increasing interest due to their potential technological application, like photo-detectors, optoelectronic devices and their promising features for quantum information processing and photonic applications. The goal of this thesis is the study of electronic and spin transport properties on quasi-one-dimensional semiconductor systems; specifically, homogenous nanowires (NWs), coupled NW s, twin-plane (TP) NWs, resonant tunneling diodes (RTDs), and quantum dot chains (QDCs). The k-p method, in particular the Luttinger Hamiltonian, was chosen to describe the effects of biaxial confinement and strain. This suggested a modulation of the ground state character that, complemented with the phonon dynamics provided by Molecular Dynamics (MD) simulations, allowed the description of the hole mobility modulation by either phonon emission or absorption. Regarding the coupled NW s system, the electron and spin transport properties affected by a Rashba spin-orbit interaction (SOI) at the joined region were unveiled through the Transfer Matrix Method (TMM). Various configurations of gate voltages (Vg), applied on the wire structure, were considered. We were able to understand the modulation of the spin transport projected in the z-direction trough the combination of the SOI and the system dimensionalities. Likewise, the combination of SOI and applied Vg gave rise to a modulation of the polarization, when the measured spin is projected in the same direction where the Rashba SOI acts, the y-direction. The transport properties of a DBS and the effect of a resistance in series was explored within the TMM to prove the nature of a bistability of the I V characteristics and its enhanced area with temperature provided by the experiment. The model indicates that increasing the resistente by decreasing the temperature, the bistable area enhances. The presence of an additional heterojunction induces a sheet charge at its interfaces. Under this configuration, the total voltage drop of the RTD changes and can be confirmed experimentally.The formation of the peculiar strain fields and their influence on the electronic structure and transport properties of a TP superlattice was systematically studied. Hence, the transport properties of both electrons and holes could be effectively tuned even in the case of T-electrons of zincblende systems, contrasting to the predicted transparency of T-electrons in heterolayered III-V semiconductor superlattices. Also, the transmission probability for holes at valence band could also be effectively modified by applying an external stress. Finally, using molecular-beam-epitaxy and skillful strain engineering, systems of In-GaAs QDCs were successfully synthesized by collaborators. The QDCs with different doping concentrations showed an anisotropic behavior of the conductance, measured along and across the QDCs, with temperature. The theoretical ID hopping model developed found that the presence of OD states shapes the anisotropic response of the conductance in this system.

Em sistemas com acoplamento spin-órbita (SO) é possível manipular eletricamente o spin do elétron via a aplicação de um campo elétrico.1 Isso permite a potencial aplicação do grau de liberdade de spin (Spintronica) no desenvolvimento de novos dispositivos e tecnologias, como por exemplo na tecnologia da informação (computação quântica).2,3 No entanto, sabe-se que a interação SO causa efeitos indesejáveis, como por exemplo a relaxação e o defasamento de spin.4 Dessa maneira, do ponto de vista de aplicações, torna-se desejável maximizar o tempo de vida do spin. Neste trabalho, investigamos a relaxação de spin dos elétrons de condução em poços quânticos com duas sub-bandas5 crescidos ao longo das direções [001] e [110] via o mecanismo de D\'yakonov-Perel\'.6 Combinando teoria de grupos, o método k.p, a aproximação da função envelope e teoria de perturbação de Löwdin obtemos um Hamiltoniano efetivo para os elétrons da banda de condução na presença das interações SO de Rashba e Dresselhaus. Aqui, diferentemente de alguns trabalhos anteriores,7,8 além de incluir o termo cúbico de Dresselhaus, também levamos em conta as contribuições devido à influência da segunda sub-banda de mais baixa energia do poço. A partir deste Hamiltoniano derivamos expressões para os tempos de relaxação do spin e analisamos como estas novas contribuições (termos do acoplamento com a segunda sub-banda) afetam os tempos de vida dos spins. Comparamos os tempos de relaxação para as direções [001] com os calculados para a direção [110]. Nossos resultados mostram que as contribuições devido à segunda sub-banda são desprezíveis para ambas as direções. Mostramos também que o tempo de relaxação para a direção [110] é mais longo que o da [001], resultado consistente com experimentos9,10 e outros trabalhos teóricos anteriores.7 / In systems with spin-orbit (SO) coupling, it is possible to electrically manipulate the electron spin via applied gate voltages.1 This allows for the potential use of the spin degree of freedom (Spintronics) in the development of new devices and technologies, for instance information technology (quantum computing).2,3 It is known however, that the SO interaction leads to the undesired effect of causing spin relaxation and spin dephasing.4 Thus from the point of view of applications, it is desirable to maximize the spin lifetimes. Here, we investigate the spin relaxation of the conduction electrons in quantum wells with two sub-bands5 grown along the [001] and [110] directions via the D\'yakonov-Perel\' mechanism.6 By combining group theory, the k.p method, the envelope function approach and the Löwdin perturbation theory, we obtain an effective Hamiltonian for the conduction electrons in the presence of the Rashba and Dresselhaus SO interactions. Differently from some early works,7,8 in addition to the cubic Dresselhaus term, we also account for the contributions arising from the second lowest sub-band of the well. We derive expressions for the spin relaxation times and analyze how the new contributions (second sub-band terms) affect the spin lifetimes. We compare the relaxation times obtained in the [001] direction with those calculated for the [110] direction. Our results show that the contributions from the second sub-band are negligible for both directions. We also find that the relaxation time in the [110] direction is longer than the one in the [001], a result consistent with experiments9,10 and earlier theoretical works.7

Un des objectifs du Femtomagnetisme est de contrôler l’aimantation des matériaux avec des impulsions laser femtoseconde. Il a été démontré qu’une réponse magnéto-optique (MO) cohérente a lieu avant la thermalisation des populations de spins dans une configuration pompe-sonde MOKE. Elle résulte du couplage cohérent spin-photon dû à l’interaction spin-orbite. Une description simplifiée de cet effet a été faite en tenant compte d’un système à huit niveaux couplés au champ laser. La cohérence MO est définie par le temps de déphasage dépendent du champ T2MO. Dans ce travail, il est montré que la réponse MO cohérente d’un grenat dopé au bismuth peut être mesurée directement avec différentes configurations de mélange à quatre ondes MO. L’importance de connaître la phase spectrale de l’impulsion pour obtenir T2MO a été étudié. Avec des impulsions de 10fs dans le proche infra-rouge, une mesure de T2MO donne (2.8+/-1)fs, c. à d., du même ordre de grandeur que le temps de déphasage des charges. / One of the goals of Femtomagnetism is to manipulate the magnetization of materials using femtosecond optical pulses. It has been shown in ferromagnetic films that a magneto-optical (MO) coherent response takes place before the thermalization of the spins populations in a pump and probe MOKE experiment. It results from the coherent spin-photon coupling mediated by the spin-orbit interaction. A simplified description of this effect has been made by considering an eight-level system coupled with the laser field. The MO coherence can be defined by the magnetic field dependent dephasing time T2MO. In the present work, it is shown that the coherent MO response of a bismuth-doped garnet can be directly measured in different degenerated MO four-wave mixing configurations. The importance of well-knowing the spectral phase of the pulse to measure T2MO was studied. Using 10fs near infra-red pulses, T2MO was shown to be (2.8+/-1)fs that is of the same order of the charges dephasing time.

The chemistry of actinides in solution is a very important aspect of the nuclear fuel cycle, especially as the energy needs of the world continue to increase. However, the radio-active nature of the actinides makes experimentation very difficult and dedicated expensive instruments are required. In addition, the disposal of radio-active waste materials requires a proper understanding of their chemistry at a molecular level. To tackle the problem, and to underpin the experimental studies, in this thesis we have studied the redox chemistry and disproportionation mechanism of actinyl complexes in solution using state-of-the art computational methods. Reduction potentials of actinyl complexes in solution have been estimated in solution using density functional theory (DFT) approaches. Solvation effects were included in the quantum chemistry calculations with the conductor like polarisable continuum model (CPCM) solvation method. First of all, we have validated our computational method by studying a variety of solute cavity definitions within the CPCM solvation model and assessed the performance of a range of DFT functionals to suitable to accurately describe the actinide chemistry in solution. Penta-valent uranyl(V) ions are unstable and readily disproportionate; in this study we have explored outer-sphere electron transfer and disproportionation mechanisms to determine the stability of these ions in solution. We have found that the process of outer-sphere disproportionation is unlikely to occur in non-aqueous solutions, such as DMSO, DMF, DCM, acetonitrile and pyridine, when the uranyl(V) ion is bound with a multi-dentate organic ligand. However, our computational results hypothesise that the presence of a trace of water in the experimental conditions can promote a disproportionation reaction by protonating the uranyl(V) ‘yl’ oxygen atoms and then the electron transfer process would proceed through either inner or outer sphere mechanism. In addition, the effect of alkali metal cations on the outer-sphere disproportionation mechanisms was also studied. Overall it has been shown that DFT can be used to accurately predict the redox properties of actinyl complexes in solution and thus contributing for an effective and efficient design of nuclear material separations, proper as well as safer radioactive waste disposal.

No description available.