Ce travail présente l'étude de la dynamique de spins d'ions Mn insérés dans des structures de CdTe de faibles dimensions. L'accent est plus particulièrement mis sur des boîtes quantiques individuelles de CdTe contenant un ion Mn unique, ce qui permet d'accéder aux interactions non perturbées de l'ion magnétique avec son environnement semi-conducteur. Nous présentons une méthode purement optique de manipulation et de lecture des états de spin de l'ion magnétique unique. Les expériences utilisent le fait que les états de spin se conservent lors d'un transfert excitonique entre proches boîtes quantiques, pour injecter un exciton polarisé dans la boîte contenant l'ion Mn afin d'orienter son spin. Les dynamiques de processus de réorientation sont observées lors de mesures résolues en temps, puis analysées via un modèle simple d'équations de taux. Un des mécanismes possible de réorientation, la recombinaison d'excitons sombres, est présenté expérimentalement, puis discuté. L'orientation optique de l'ion Mn est aussi utilisée pour étudier les relaxations spin-réseau d'un ion magnétique isolé sous faibles et sous forts champs magnétiques. Ce travail décrit aussi les phénomènes présents pour des champs magnétiques nuls ou faibles dans des systèmes de moments magnétiques plus grands (puits et boîtes quantiques contenant plusieurs ions Mn). Une nouvelle technique expérimentale, basée sur des impulsions magnétiques rapides, nous permet d'étudier la dynamique de spin des ions Mn en l'absence de champ magnétique et ce, avec une résolution temporelle de l'ordre de la nanoseconde. Nous observons une rapide décroissance de la magnétisation après une impulsion magnétique. Le phénomène est décrit en terme de couplage hyperfin avec le spin nucléaire des ions Mn. Cet effet est particulièrement sensible à toute anisotropie, notamment celles introduites par un gaz de trous ou par les contraintes du réseau. L'application d'un champ magnétique externe supprime les dynamiques rapides dans les puits quantiques magnétiques dilués et des phénomènes plus commun de relaxation lente spin-réseau sont alors observés. Il est toutefois surprenant que les boîtes quantiques avec un grand nombre d'ions Mn présentent ces dynamiques de spin rapides même après application d'un champ magnétique allant jusqu'à 0.5 T. Ce processus rapide pourrait venir des interactions spin-spin des ions Mn, en particulier si leur distribution spatiale n'est pas régulière à l'intérieur de la boîte. / This work is devoted to the studies of spin dynamics of magnetic Mn ions embedded in low-dimensional CdTe-based nanostructures. A particular emphasis is placed on the system of single CdTe quantum dots with single Mn ions, which give an insight into unperturbed interactions of magnetic ion with its semiconductor environment. A method of all-optical manipulation and readout of the spin state of a single magnetic ion is presented. The experiment exploits the spin-conserving exciton transfer between neighbouring quantum dots to inject polarized exitons into the dot with the Mn ion so as to orient its spin. The dynamics of the orientation process is measured in a time-resolved experiment and described with a simple rate equation model. One of possible orientation mechanisms - the dark excitons recombination - is discussed and shown experimentally. The optical orientation of the Mn ion is also used to investigate the spin-lattice relaxation of an isolated magnetic ion in low and high magnetic field. The work also addresses phenomena occurring in low and zero magnetic field in large systems of magnetic moments - quantum wells and quantum dots containing Mn ions. New experimental technique of fast magnetic pulses is used to investigate the Mn spin dynamics in the absence of magnetic field with nanosecond resolution. After the pulse of magnetic field, a fast decay of the magnetization is observed. The experimental findings are described in terms of hyperfine coupling with the nuclear spin of the Mn ions. The effect is highly sensitive to the presence of an anisotropy, particularly that introduced by hole gas and by strain. Application of the external magnetic field suppresses the fast dynamics in diluted magnetic quantum wells and a well known slow spin-lattice relaxation is observed. Surprisingly, quantum dots with many Mn ions show fast spin dynamics even after application of external field up to 0.5 T. The fast process may origin from the spin-spin interaction between the magnetic ions, especially if their spatial distribution within the dot is not uniform.

Ce travail a porté sur les propriétés d'éléments minces de métaux ferromagnétiques étudiées à petite échelle (µm) et à<br />haute fréquence (GHz). Dans ce but, un spectromètre hyperfréquence à antennes micrométriques a été mis au point. Cet<br />instrument a été utilisé pour explorer deux problématiques différentes. Pour un film continu, d'abord, nous avons réalisé des<br />expériences d'émission-réception d'ondes de spin. Ces résultats nous ont permis de caractériser les processus de<br />transduction et de relaxation d'ondes magnétostatiques progressives. Nous avons également étudié des rubans de largeur<br />micrométrique, pour lesquels l'équilibre lui-même est inhomogène. Nous avons interprété leur réponse hyperfréquence en<br />termes de transitions de phase micromagnétiques et en termes de confinement d'ondes de spin.

<p>Theoretical studies based on first-principles theory are presented for a number of different magnetic systems. The first part of the thesis concerns spin dynamics and the second part concerns properties of magnetic multilayers. The theoretical treatment is based on electronic structure calculations performed by means of density functional theory.</p><p>A method is developed for simulating atomistic spin dynamics at finite temperatures, which is based on solving the equations of motion for the atomic spins by means of Langevin dynamics. The method relies on a mapping of the interatomic exchange interactions from density functional theory to a Heisenberg Hamiltonian. Simulations are performed for various magnetic systems and processes beyond the reach of conventional micromagnetism. As an example, magnetization dynamics in the limit of large magnetic and anisotropy fields is explored. Moreover, the method is applied to studying the dynamics of systems with complex atomic order such as the diluted magnetic semiconductor MnGaAs and the spin glass alloy CuMn. The method is also applied to a Fe thin film and a Fe/Cr/Fe trilayer system, where the limits of ultrafast switching are explored. Current induced magnetization dynamics is investigated by calculating the current induced spin-transfer torque by means of density functional theory combined with the relaxation time approximation and semi-classical Boltzmann theory. The current induced torque is calculated for the helical spin-density waves in Er and fcc Fe, where the current is found to promote a rigid rotation of the magnetic order.</p><p>Properties of magnetic multilayers composed of magnetic and nonmagnetic layers are investigated by means of the Korringa-Kohn-Rostocker interface Green's function method. Multilayer properties such as magnetic moments, interlayer exchange coupling and ordering temperatures are calculated and compared with experiments, with focus on understanding the influence of interface quality. Moreover, the influence on the interlayer exchange coupling of alloying the nonmagnetic spacer layers with small amounts of a magnetic impurity is investigated.</p>

Theoretical studies based on first-principles theory are presented for a number of different magnetic systems. The first part of the thesis concerns spin dynamics and the second part concerns properties of magnetic multilayers. The theoretical treatment is based on electronic structure calculations performed by means of density functional theory. A method is developed for simulating atomistic spin dynamics at finite temperatures, which is based on solving the equations of motion for the atomic spins by means of Langevin dynamics. The method relies on a mapping of the interatomic exchange interactions from density functional theory to a Heisenberg Hamiltonian. Simulations are performed for various magnetic systems and processes beyond the reach of conventional micromagnetism. As an example, magnetization dynamics in the limit of large magnetic and anisotropy fields is explored. Moreover, the method is applied to studying the dynamics of systems with complex atomic order such as the diluted magnetic semiconductor MnGaAs and the spin glass alloy CuMn. The method is also applied to a Fe thin film and a Fe/Cr/Fe trilayer system, where the limits of ultrafast switching are explored. Current induced magnetization dynamics is investigated by calculating the current induced spin-transfer torque by means of density functional theory combined with the relaxation time approximation and semi-classical Boltzmann theory. The current induced torque is calculated for the helical spin-density waves in Er and fcc Fe, where the current is found to promote a rigid rotation of the magnetic order. Properties of magnetic multilayers composed of magnetic and nonmagnetic layers are investigated by means of the Korringa-Kohn-Rostocker interface Green's function method. Multilayer properties such as magnetic moments, interlayer exchange coupling and ordering temperatures are calculated and compared with experiments, with focus on understanding the influence of interface quality. Moreover, the influence on the interlayer exchange coupling of alloying the nonmagnetic spacer layers with small amounts of a magnetic impurity is investigated.

This thesis is a study of the static and dynamic behavior of the magne-tization in spin-flop bi-layers, which consist of two soft ferromagnetic layerscoupled by dipolar forces through a thin nonmagnetic spacer. The focus ofthe work is three fold: collective spin dynamics in the anti-parallel groundstate; resonant switching in the presence of thermal agitation; and static anddynamic behavior of the system in the vortex-pair state, with a particularemphasis on the interlayer core-core interaction. Two collective spin-flop resonance modes are observed and interpreted asacoustical and optical spin precessions, in which the moments of the two lay-ers oscillate in phase and out of phase, respectively. An analytical macrospinmodel is developed to analyze the experimental results and is found to ac-curately predict the resonance frequencies and their field dependence in thelow-field anti-parallel state and the high-field near saturated state. A micro-magnetic model is developed and successfully explains the static and dynamicbehavior of the system in the entire field range, including the C- and S-typespin-perturbed scissor state of the bi-layer at intermediate fields. The optical spin-flop resonance at 3-4 GHz is used to demonstrate resonantswitching in the system, in the range of the applied field where quasi-staticswitching is forbidden. An off-axis field of relatively small amplitude canexcite large-angle scissor-like oscillations at the optical resonance frequency,which can result in a full 180-degree reversal, with the two moments switchingpast each other into the mirror anti-parallel state. It is found that the switch-ing probability increases with increasing the duration of the microwave fieldpulse, which shows that the resonant switching process is affected by thermalagitation. Micromagnetic modeling incorporating the effect of temperature isperformed and is in good agreement with the experimental results. Vortex pair states in spin-flop bi-layers are produced using high amplitudefield pulses near the optical spin resonance in the system. The stable vortex-pair states, 16 in total, of which 4 sub-classes are non-degenerate in energy, areidentified and investigated using static and dynamic applied fields. For AP-chirality vortex-pair states, the system can be studied while the two vortexcores are coupled and decoupled in a single field sweep. It is found thatthe dynamics of the AP-chirality vortex pairs is critically determined by thepolarizations of the two vortex cores and the resulting attractive or repulsivecore-core interaction. The measured spin resonance modes in the system areinterpreted as gyrational, rotational, and vibrational resonances with the helpof the analytical and micromagnetic models developed herein. A significant effort during this project was made to build two instrumentsfor surface and transport characterization of magnetic nanostructures: a high-current Scanning Tunneling Microscope for studying transport in magneticpoint contacts, and a Current In Plane Tunneling instrument for characteriz-ing unpatterned magnetic tunnel junctions. The design and implementationof the instruments as well as the test data are presented. / QC 20101209

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.

The magnetocaloric effect (MCE) is the temperature change in a magnetic material due to a change in an applied magnetic field. How the MCE behaves in different magnetic materials and at different phase transitions is fundamental to understand. The driver of the MCE is a change in entropy which has multiple contributions: magnetic, lattice, and electron. In this thesis the MCE is studied in a simple antiferromagnetic (AFM) model andin a realistic noncollinear spin glass Neodymium model using Monte Carlo and Atomistic Spin Dynamics simulations. For the simple AFM system, no clear results were achieved, indicating that MCE in AFM materials is not due to a change solely in the magnetic entropy. For the complex magnetic material Nd, a more clear result is seen, indicating that frustration in the system might be important to the MCE in noncollinear materials. Nd results also signify more phase transitions than previously reported.

In recent years, spin relaxation, injection, and manipulation in semiconductors have attracted considerable interest because of several potential applications in "spintronic" devices and the necessity to understand and control spin-based phenomena. In light of the growing interest in spin-related phenomena and devices, there is now renewed interest in the science and engineering of narrow gap semiconductors (NGS). NGS based heterostructures are particularly interesting for spintronic applications due to their large spin-orbit coupling, which leads to considerable zero-field spin splitting. NGS are also candidates for electronic applications, such as high-speed and low-power microprocessors; as reported recently by Intel. Furthermore, as switching rates in electronic devices are pushed to even higher frequencies, it is important to understand dynamics in semiconductors such as NGS on femtosecond time-scales. In this thesis, time-resolved studies of magnetic and non-magnetic NGS using ultrafast-laser spectroscopy techniques such as pump-probe spectroscopy and magneto-optical Kerr/Faraday effect, are reported. Our samples include: InSb-based quantum wells with different confinement potentials; InMnSb films, the newest III-V ferromagnetic semiconductors; and InAs films. The samples for these studies have been provided by the groups of Prof. Santos at the University of Oklahoma, Prof. Furdyna at the University of Notre Dame, and Prof. Guido at Virginia Tech. The objectives in this thesis have been to: a) understand charge/spin dynamics in NGS with novel confinement potentials, b) probe the effect of magnetic impurities on the spin/charge dynamics, and c) develop concepts for spin based device applications. Several specific questions and concepts have been addressed including: the effect of large spin-orbit interaction in NGS on the dynamics, how large Rashba spin splitting in these materials affect the spin coherence life time, and carrier/spin dynamics in ferromagnetic semiconductor structures. / Ph. D.

The outcome of chemical reactions proceeding via radical pair (RP) intermediates can be influenced by the magnitude and direction of applied magnetic fields, even for interaction strengths far smaller than the thermal energy. Sensitivity to Earth-strength magnetic fields has been suggested as a biophysical mechanism of animal magnetoreception and this thesis is concerned with simulations of the effects of such weak magnetic fields on RP reaction yields. State-space restriction techniques previously used in the simulation of NMR spectra are here applied to RPs. Methods for improving the efficiency of Liouville-space spin dynamics calculations are presented along with a procedure to form operators directly into a reduced state-space. These are implemented in the spin dynamics software Spinach. Entanglement is shown to be a crucial ingredient for the observation of a low field effect on RP reaction yields in some cases. It is also observed that many chemically plausible initial states possess an inherent directionality which may be a useful source of anisotropy in RP reactions. The nature of the radical species involved in magnetoreception is investigated theoretically. It has been shown that European Robins are disorientated by weak radio-frequency (RF) fields at the frequency corresponding to the Zeeman splitting of a free electron. The potential role of superoxide and dioxygen is investigated and the anisotropic reaction yield in the presence of a RF-field, without a static field, is calculated. Magnetic field effect data for Escherichia coli photolyase and Arabidopsis thaliana cryptochrome 1, both expected to be magnetically sensitive, are satisfactorily modelled only when singlet-triplet dephasing is included. With a view to increasing the reaction yield anisotropy of a RP magnetoreceptor, a brief study of the amplification of the magnetic field experienced by a RP from nearby magnetite particles is presented. Finally in a digression from RPs, Spinach is used to determine the states expected to be immune from relaxation and therefore long-lived in NMR experiments on multi-spin systems.

Nous avons obtenu des angles de rotation Faraday (RF) allant jusqu'à 19° par orientation optique d'un gaz d'électrons dans GaAs de type n inclus dans une microcavité (Q=19000), sans champ magnétique. Cette forte rotation est obtenue en raison des multiples allers-retours de la lumière dans la cavité. Nous avons également démontré la commutation optique rapide de la RF à l'échelle sub-microseconde en échantillonnant le signal de RF sous excitation impulsionnelle mono-coup. De la dépolarisation de la RF en champ magnétique transverse, nous avons déduit un temps de relaxation de spin de 160 ns. Le concept de section efficace de RF, coefficient de proportionnalité entre l'angle RF, la densité de spin électronique, et le chemin parcouru, a été introduit. La section efficace de RF, qui définit l'efficacité du gaz d'électrons à produire une RF, a été estimée quantitativement, et comparée avec la théorie. Nous avons également démontré la possibilité de mesurer de manière non destructive l'aimantation nucléaire dans GaAs-n, via la RF amplifiée par la cavité. Contrairement aux méthodes existantes, cette détection ne nécessite pas la présence d'électrons hors équilibre. Par cette technique nous avons étudié la dynamique de spin nucléaire dans GaAs-n avec différents dopages. Contrairement à ce qu'on pourrait attendre, le déclin de la RF nucléaire est complexe et consiste en deux composantes ayant des temps de relaxation très différents. Deux effets à l'origine de la RF nucléaire sont identifiés: le splitting de spin de la bande de conduction, et la polarisation en spin des électrons localisés, tous deux induits par le champ Overhauser. Le premier effet domine la RF nucléaire dans les deux échantillons étudiés, tandis que la RF induite par les électrons localisés n'a été observée que dans l'échantillon métallique. / We obtained Faraday rotation (FR) up to 19° by using optical orientation of electron gas in n-doped bulk GaAs confined in a microcavity (Q=19000), in the absence of magnetic field. This strong rotation is achieved because the light makes multiple round trips in the microcavity. We also demonstrated fast optical switching of FR in sub-microsecond time scale by sampling the FR in a one-shot experiment under pulsed excitation. From the depolarization of FR by a transverse magnetic field, we deduce electron spin relaxation time of about 160 ns. A concept of FR cross-section as a proportionality coefficient between FR angle, electron spin density and optical path is introduced. This FR cross-section which defines the efficiency of spin polarized electrons in producing FR was estimated quantitatively and compared with theory. We also demonstrated non-destructive measurement of nuclear magnetization in n-GaAs via cavity enhanced FR. In contrast with the existing optical methods, this detection scheme does not require the presence of detrimental out-of-equilibrium electrons. Using this technique, we studied nuclear spin dynamics in n-GaAs with different doping concentrations. Contrary to simple expectation, the nuclear FR is found to be complex, and consists of two components with vastly different time constants. Two effects at the origin of FR have been identified: the conduction band spin splitting and the localized electron spin polairzation both induced by the Overhauser field. The first effect dominates the FR in both studied samples, while the FR induced by the localized electrons has been observed only in the metallic sample.