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.

Neste trabalho exploramos o uso de sequências de pulsos de Ressonância Magnética Nuclear de Estado Sólido (RMN-ES) que utilizam o acoplamento dipolar magnético heteronuclear para o estudo de reorientações de segmentos moleculares no regime intermediário, testando-as em amostras modelo a fim de verificar suas eficiências. Paralelamente, simulações numéricas foram realizadas juntamente com cálculos analíticos para a melhor compreensão dos efeitos experimentais observados nessas sequências de pulsos. A primeira proposição, baseia-se no uso de Perfis de Hartmann-Hahn obtidos utilizando a Transferência de Polarização Cruzada (CPMAS) sob desacoplamento dipolar homonuclear Lee-Goldburg (LG), usando a interação dipolar heteronuclear como sonda do movimento molecular. A segunda proposição consiste em uma variação das técnicas DIPSHIFT e Time Constant recDIPSHIFT , o T2-recDIPSHIFT, segundo a qual, em condições favoráveis, é possível quantificar parâmetros dinâmicos relacionados aos movimentos moleculares no regime intermediário de sistemas fracamente acoplados pela interação dipolar magnética heteronuclear ou com geometrias de movimento de baixa amplitude. Por fim, propomos um novo método analítico para quantificação de parâmetros dinâmicos em experimentos de Separação de campo locais (SLF), baseado no método de Anderson-Weiss. Demonstramos a precisão do método analítico comparando curvas de Time Constant recDIPSHIFT para diversas taxas e geometrias de movimento obtidas pela aproximação analítica e pelo cálculo exato, além de efetuar um teste experimental em uma amostra modelo. / In the present work we explore the use of Solid State Nuclear Magnetic Resonance (NMR) pulse sequences which use the heteronuclear dipolar magnetic coupling to study local rotations of molecular groups in the intermediate-regime of motion, testing them in standard samples in order to verify their efficiency. Simultaneously, numerical simulations and analytical calculations were performed to understand the experimental artifacts observed in these new pulse sequences. The first proposal, based on using Hartmann-Hahn matching profiles obtained by using the Cross Polarization transfer (CPMAS) under Lee-Goldburg homonuclear decoupling (LG), utilizing the heteronuclear dipolar interaction as probe of the molecular motion. The second proposal consists in a variation of DIPSHIFT and Time Constant recDIPSHIFT pulse sequences, dubbed T2 - recDIPSHIFT, whereby, in favorable conditions, it is possible to quantify molecular dynamic parameters of systems weakly coupled by heteronuclear dipolar interaction or to probe small-amplitude molecular motions. Finally, we proposed a new analytical method to describe Separated Local Field experiments (SLF), based upon the Anderson-Weiss approximation. We demonstrate the accuracy of the method comparing the Time Constant recDIPSHIFT curves for several rates and geometries of motion obtained by the analytical approximation and exact calculation, besides an experimental test has been performed in a model sample.

Ce travail de thèse porte sur l'étude par la résonance paramagnétique électronique (RPE) des sels à transfert de charge quasi-unidimensionnels (TMTTF)$ {2}$X (X=AsF$ {6}$, PF$ {6}$, SbF$ {6}$), matériaux modèles de chaînes de spins quantiques. Tout d'abord, nous avons examiné en onde continue et sur une large gamme de température et de fréquence, la phase d'ordre de charge déjà observée dans ces matériaux en dessous de la température T$ {CO}$. Nous avons mis en évidence deux nouveaux phénomènes à T < T$ {CO}$: la rotation des axes principaux du facteur g et une modification structurale liée à un dédoublement de la maille cristallographique. Un calcul de chimie quantique a été réalisé à l'aide de la méthode DFT confirmant nos résultats expérimentaux. Dans la seconde partie de ces travaux de thèse, nous avons présenté les résultats obtenus par RPE en onde continue et en onde pulsée sur l'étude des défauts corrélés dans les systèmes à chaînes de spins. En onde continue, nous avons détecté pour la première fois une raie RPE fine à basse température, suggérant la présence de défauts corrélés ayant les caractéristiques de solitons. Les mesures par RPE pulsée nous ont permis d'observer les premières oscillations de Rabi de solitons piégés et de déterminer leur caractère robuste. Ces derniers résultats offrent une approche alternative aux qubits à base de spins pour le traitement de l’information quantique. / This thesis focuses on the study by Electron Paramagnetic Resonance (EPR) of the quasi-one-dimensional charge transfer salts (TMTTF)$ {2}$X (X=AsF$ {6}$, PF$ {6}$, SbF$ {6}$), model materials of quantum spin chains. First, we have examined in continuous wave and on a wide range of temperature and frequency, the charge-ordered phase already observed in these materials below the temperature T$ {CO}$. We have identified two new phenomena at T <T$ {CO}$: the rotation of the principal axes of the g factor and a structural change related to a doubling of the unit cell parameter. A quantum chemical calculation was carried out using DFT confirming our experimental results. In the second part of the thesis, we have presented the results obtained by EPR in continuous wave and pulsed wave on the correlated defects study in spin chain systems. In continuous wave, we have detected for the first time a narrow EPR line at low temperature, suggesting the presence of correlated defects having the characteristics of solitons. The pulsed EPR measurements allowed us to observe the first Rabi oscillations of trapped solitons and to determine their robust character. These latter results offer an alternative approach for spin qubits in quantum information processing.

L'étude des excitations magnétiques de faible amplitude existant dans des films minces à aimantation non uniforme dans la gamme des hautes fréquences, typiquement entre quelques dizaines de MHz et quelques dizaines de GHz, constitue le sujet de ce mémoire. Le cas idéal de films magnétiques possédant une anisotropie perpendiculaire et présentant une configuration d'équilibre de l'aimantation sous forme de rubans parallèles et périodiques est étudié en détail. Dans le cas de films à forte anisotropie perpendiculaire, les spectres théoriques de susceptibilité dynamique calculés à l'aide de modèles analytiques puis, à partir de simulations numériques 2D de micromagnétisme dynamique, font apparaître des excitations localisées soit à l'intérieur des domaines magnétiques soit à l'intérieur des parois magnétiques. Ces résultats ont été comparés de façon satisfaisante avec des résultats expérimentaux issus de mesures de résonance ferromagnétique réalisées sur des films monocristallins de grenats ferrimagnétiques. Toutefois, les largeurs de raie expérimentales associées aux excitations de parois excèdent celles calculées en utilisant le terme dissipatif de Gilbert. Dans le cas de films à faible anisotropie perpendiculaire, les spectres théoriques de susceptibilité dynamique présentent de multiples excitations magnétiques liées à la forte hétérogénéité des configurations d'équilibre de l'aimantation de type rubans faibles. Les analyses modales effectuées à partir des simulations micromagnétiques dynamiques indiquent l'existence de modes de surface et de volume localisés dans différentes régions de spins à l'intérieur du film. L'influence de différents paramètres (anisotropie perpendiculaire, épaisseur du film, champ magnétique statique) sur les principales caractéristiques des spectres (nombre de résonances, fréquences de résonance, intensités et largeurs de raie) est ensuite étudiée. Ces simulations micromagnétiques dynamiques permettent d'interpréter des spectres expérimentaux complexes de perméabilité dynamique mesurés sur des films ferromagnétiques amorphes. Quelques perspectives concernant la dynamique de l'aimantation de faible amplitude dans différents objets magnétiques sont ensuite présentées.

The topic of this Thesis is magnetization dynamics on atomic length scales. A computational scheme, Atomistic Spin Dynamics, based on density functional theory, the adiabatic approximation and the atomic moment approximation is presented. Simulations are performed for chemically disordered systems, antiferromagnets and ferrimagnets and also systems with reduced dimensionality The autocorrelation function of the archetypical spin glass alloy CuMn is sampled in simulations following a quenching protocol. The aging regime can be clearly identified and the dependence of the relaxation on the damping parameter is investigated. The time evolution of pair correlation and autocorrelation functions has been studied in simulations of the dilute magnetic semiconductor GaMnAs. The dynamics reveal a substantial short ranged magnetic order even at temperatures at or above the ordering temperature. The dynamics for different concentrations of As antisites are discussed. Antiferromagnets offer opportunities for ultrafast switching, this is studied in simulations of an artificial antiferromagnet. For the right conditions, the cooperative effect of applied field torque and and the torque from the other sublattice enables very fast switching. The dynamics of bcc Fe precessing in a strong uniaxial anisotropy are investigated. It is demonstrated that the magnetization can shrink substantially due to a spin wave instability. The dynamics of a two-component model ferrimagnet at finite temperature are investigated. At temperatures where the magnetic system is close to the magnetic and angular momentum compensations points of the ferrimagnet, the relaxation in a uniaxial easy exis anisotropy resembles results in recent experiments on ferrimagnetic resonance. The different cases of uniaxial or colossal magnetic anisotropy in nanowires at different temperatures are compared. The magnon softening in a ferromagnetic monolayer is investigated, giving results that compare well with recent experiments. The effect of lattice relaxation can be treated in first principles calculations. Subsequent simulations captures the softening of magnons caused by reduced dimensionality and temperature. / Felaktigt tryckt som Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology 706

Dans cette thèse, nous proposons d’explorer la relation entre transport électronique et dynamique d’aimantation afin de mieux comprendre certaines propriétés des films minces de métaux ferromagnétiques. Afin d’extraire l’influencede la diffusion des électrons par les surfaces sur les résistivités dépendantes du spin, des séries d’épaisseur de films de permalloy (Ni80Fe20) ont été déposées et étudiées. En plus de mesures électriques et magnétiques conventionnelles,nous avons réalisé une étude détaillée de la propagation des ondes de spin dans ces films. La technique du décalage Doppler d’ondes de spin induit par un courant électrique a été utilisée pour extraire le degré de polarisation en spin du courant électrique. Nous avons observé que ce degré de polarisation décroît lorsque l’épaisseur du film décroît, ce qui suggère que les surfaces contribuent aux résistivités dépendantes du spin et qu’elles ont tendance à dépolariser le courant électrique. / In this thesis, the interplay between electron transport and magnetization dynamics is explored in order to access to fundamental properties of ferromag- netic metal thin films. With the aim of extracting the influence of the electron surface scattering on the spin-dependent resistivities, thickness series of permal-loy (Ni80Fe20) films were grown and studied. In addition to standard electrical and magnetic measurements, a detailed study of the propagation of spin waves along these films was performed. Resorting to the current-induced spin-wave Doppler shift technique, the degree of spin-polarization of the electrical current was extracted. This degree of spin-polarization was found to decrease when the film thickness decreases, which suggests that the film surfaces contribute to the spin dependent resistivities and tend to depolarize the electrical current.

Neste trabalho exploramos o uso de sequências de pulsos de Ressonância Magnética Nuclear de Estado Sólido (RMN-ES) que utilizam o acoplamento dipolar magnético heteronuclear para o estudo de reorientações de segmentos moleculares no regime intermediário, testando-as em amostras modelo a fim de verificar suas eficiências. Paralelamente, simulações numéricas foram realizadas juntamente com cálculos analíticos para a melhor compreensão dos efeitos experimentais observados nessas sequências de pulsos. A primeira proposição, baseia-se no uso de Perfis de Hartmann-Hahn obtidos utilizando a Transferência de Polarização Cruzada (CPMAS) sob desacoplamento dipolar homonuclear Lee-Goldburg (LG), usando a interação dipolar heteronuclear como sonda do movimento molecular. A segunda proposição consiste em uma variação das técnicas DIPSHIFT e Time Constant recDIPSHIFT , o T2-recDIPSHIFT, segundo a qual, em condições favoráveis, é possível quantificar parâmetros dinâmicos relacionados aos movimentos moleculares no regime intermediário de sistemas fracamente acoplados pela interação dipolar magnética heteronuclear ou com geometrias de movimento de baixa amplitude. Por fim, propomos um novo método analítico para quantificação de parâmetros dinâmicos em experimentos de Separação de campo locais (SLF), baseado no método de Anderson-Weiss. Demonstramos a precisão do método analítico comparando curvas de Time Constant recDIPSHIFT para diversas taxas e geometrias de movimento obtidas pela aproximação analítica e pelo cálculo exato, além de efetuar um teste experimental em uma amostra modelo. / In the present work we explore the use of Solid State Nuclear Magnetic Resonance (NMR) pulse sequences which use the heteronuclear dipolar magnetic coupling to study local rotations of molecular groups in the intermediate-regime of motion, testing them in standard samples in order to verify their efficiency. Simultaneously, numerical simulations and analytical calculations were performed to understand the experimental artifacts observed in these new pulse sequences. The first proposal, based on using Hartmann-Hahn matching profiles obtained by using the Cross Polarization transfer (CPMAS) under Lee-Goldburg homonuclear decoupling (LG), utilizing the heteronuclear dipolar interaction as probe of the molecular motion. The second proposal consists in a variation of DIPSHIFT and Time Constant recDIPSHIFT pulse sequences, dubbed T2 - recDIPSHIFT, whereby, in favorable conditions, it is possible to quantify molecular dynamic parameters of systems weakly coupled by heteronuclear dipolar interaction or to probe small-amplitude molecular motions. Finally, we proposed a new analytical method to describe Separated Local Field experiments (SLF), based upon the Anderson-Weiss approximation. We demonstrate the accuracy of the method comparing the Time Constant recDIPSHIFT curves for several rates and geometries of motion obtained by the analytical approximation and exact calculation, besides an experimental test has been performed in a model sample.

No description available.

Les propriétés magnétiques des matériaux sont fortement connectées à leur structure cristallographique. Nous proposons un modèle atomique de la dynamique d'aimantation capable de rendre compte de cette magnétoélasticité. Bien que ce travail s'inscrive dans une thématique générale de l'étude des matériaux magnétiques en température, nous la particularisons à un seul élément, le Cobalt. Dans ce modèle effectif, les atomes sont décrits par 3 vecteurs classiques qui sont position, impulsion et spin. Ils interagissent entre eux via un potentiel magnéto-mécanique ad hoc. On s'intéresse tout d'abord à la dynamique de spin atomique. Cette méthode permet d'aborder simplement l'écriture des équations d'évolution d'un système atomique de spins dans lequel la position et l'impulsion des atomes sont gelées. Il est toutefois possible de définir une température de spin permettant de développer naturellement une connexion avec un bain thermique. Montrant les limites d'une approche stochastique, nous développons une nouvelle formulation déterministe du contrôle de la température d'un système à spins.Dans un second temps, nous développons et analysons les intégrateurs géométriques nécessaires au couplage temporel de la dynamique moléculaire avec cette dynamique de spin atomique. La liaison des spins avec le réseau est assurée par un potentiel magnétique dépendant des positions des atomes. La nouveauté de ce potentiel réside dans la manière de paramétrer l'anisotropie magnétique qui est la manifestation d'un couplage spin-orbite. L'écriture d'un modèle de paires étendu de l'anisotropie permet de restituer les constantes de magnétostriction expérimentales du hcp-Co. En considérant un système canonique, où pression et température sont contrôlées, nous avons mis en évidence la transition de retournement de spin si particulière au Co vers 695K.Nous finissons par l'étude des retournements d'aimantation super-paramagnétiques de nanoplots de Co permettant de comparer ce couplage spin-réseau aux mesures récentes. / The magnetic properties of materials are strongly connected to their crystallographic structure. An atomistic model of the magnetization dynamics is developed which takes into account magneto-elasticity. Although this study is valid for all magnetic materials under temperatures, this study focuses only on Cobalt. In our effective model, atoms are described by three classical vectors as position, momentum and spin, which interact via an ad hoc magneto-mechanical potential.The atomistic spin dynamics is first considered. This method allows us to write the evolution equations of an atomic system of spins in which positions and impulsions are first frozen. However, a spin temperature is introduced to develop a natural connection with a thermal bath. Showing the limits of the stochastic approach, a genuine deterministic approach is followed to control the canonical temperature in this spin system.In a second step, several geometrical integrators are developed and analyzed to couple together both the molecular dynamics and atomic spin dynamics schemes. The connection between the spins and the lattice is provided by the atomic positions dependence of the magnetic potential. The novelty of this potential lies in the parameterization of the magnetic anisotropy which originates in the spin-orbit coupling. Using a dedicated pair model of anisotropy, the magnetostrictive constants of hcp-Co are restored. In a canonical system where pressure and temperature are controlled simultaneously, the transition of rotational magnetization of Co is found.Finally the magnetization reversals of super-paramagnetic Co nanodots is studied to quantify the impact of spin-lattice coupling respectively to recent measurements.

Carrier, spin, charge current, and spin current injection by one- and two-color optical schemes are investigated within 30-band k·p theory. Parameters of the band model are optimized to give full-Brillouin zone band structures for GaAs and Ge that give accurate Γ-point effective masses and gyromagnetic factors and give access to the L valley, and to the E₁ and E₁+Δ₁ critical points in the linear optical absorption. Calculations of one- and two-photon carrier and spin injection and two-color current injection are performed for excitation energies in the range of 0—4 eV in GaAs and 0—3.5 eV in Ge. Significant spin and spin current injection occurs with 30% spin polarization in GaAs and Ge at photon energy matching the E₁ critical point. Further, the anisotropy and disparity of the current injection between parallel and perpendicular linearly-polarized beam configurations are calculated. For light propagating along a <111> crystal axis, anisotropic contributions in coherent current control and two-photon spin injection give rise to normal current components and in-plane spin components. In Ge, contributions from the holes to spin, electrical current, and spin current injection are investigated. Optical orientation results in 83% spin-polarized holes at the band edge. The effects of carrier dynamics in Ge are treated within a rate-equation model. The detection of spin dynamics in a pump-probe setup is considered, and the Fermi-factor approach is justified for electrons but not for holes. Carrier and current injection are further investigated in single-layer and bilayer graphene within the tight-binding model. In single-layer graphene, the linear-circular dichroism in two-photon absorption yields an absorption coefficient that is twice as large for circularly polarized light compared to linearly polarized light. Coherent current injection is largest for co-circularly polarized beams and zero for cross-circularly polarized beams. For linearly polarized beams, the magnitude of the injected current is independent of beam polarizations. In contrast, the injected current in bilayer graphene shows disparity between parallel and perpendicular configurations of the beams. The resulting angular dependence of the current is a macroscopic, measurable consequence of interlayer coupling in the bilayer.