Nanoscale materials behave differently than their bulk counterparts due, in part, to the reduced length scales and the increased surface to core atom ratio. As the length scales decrease, the surface atoms become increasingly important as they make up a larger percentage of the total number of atoms. These surface atoms have magnetic properties that differ from the core atoms due to a surface anisotropy that alters the interparticle, intraparticle, and exchange interactions. In this work, we have synthesized three different nanoscale systems that will allow us to explore the physics of the different interactions. Cu/gamma-Fe2O3 core/shell nanoparticles were chosen because the gamma-Fe2O3 cores have vacancies in their B-sites, broken coordination at the surface, and experience superexchange interactions. As a comparison, multiphase undoped and V-doped SiO2/FeCo nanoparticles were chosen as these nanoparticles do not suffer from vacancies or surface disorder and experience both direct exchange interactions from the nanoparticle core and superexchange interactions between the FeCo core and the metal silicate interfacial phase. Finally, Fe nanocrystallites were grown in a Cu matrix as they present no vacancies or surface disorder, and they are single phase. We observed that the interfacial phases that form in these core/shell and nanocrystallite/matrix nanoscale systems alters significantly the physics of the magnetism. The overall magnetic properties, the elemental magnetism, and the atomic magnetism were all observed to be altered by this interfacial phase, along with the interparticle and intraparticle interactions. In addition, the thickness of this interfacial phase, and thus the strength of its affect, was controlled by controlling the thickness of the shells or the amount of intermixing in the case of the nanostructured thin film. / February 2016

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<p>Magnetic properties of selected compounds and superlattices have been experimentally studied using SQUID (superconducting quantum interference device) and VSM (vibrating sample magnetometer) magnetometry, neutron diffraction and Mössbauer spectroscopy measurements combined with theoretical <i>ab initio</i> calculations. </p><p>The magnetic compounds (Fe_1-xM_x)₃P, M=Co or Mn have been studied extensively. It was found that Co can substitute Fe up to <i>x</i>=0.37. Increasing the Co content leads to a reduction of the Curie temperature and the magnetic moment per metal atom. Mn can substitute Fe up to<i> x</i>=0.25 while Fe can be substituted into Mn₃P to 1-<i>x</i>=0.33. On the iron rich side, the drop in Curie temperature and magnetic moment when increasing the Mn content is more rapid than for Co substitution. On the manganese rich side an antiferromagnetic arrangement with small magnetic moments was found. </p><p>The interlayer exchange coupling and the magnetocrystalline anisotropy energy of Fe/V superlattices were studied. The coupling strength was found to vary with the thickness of the iron layers. To describe the in-plane four-fold anisotropy, the inclusion of surface terms proved necessary. </p><p>The in-plane four fold anisotropy was also studied in a series of Fe/Co superlattices, where the thickness of the Co layers was kept thin so that the bcc structure could be stabilized. Only for samples with a large amount of iron, the easy axis was found to be [100]. The easy axis of bulk bcc Co was therefor suggested to be [111]. </p>

Magnetic properties of selected compounds and superlattices have been experimentally studied using SQUID (superconducting quantum interference device) and VSM (vibrating sample magnetometer) magnetometry, neutron diffraction and Mössbauer spectroscopy measurements combined with theoretical ab initio calculations. The magnetic compounds (Fe1-xMx)3P, M=Co or Mn have been studied extensively. It was found that Co can substitute Fe up to x=0.37. Increasing the Co content leads to a reduction of the Curie temperature and the magnetic moment per metal atom. Mn can substitute Fe up to x=0.25 while Fe can be substituted into Mn3P to 1-x=0.33. On the iron rich side, the drop in Curie temperature and magnetic moment when increasing the Mn content is more rapid than for Co substitution. On the manganese rich side an antiferromagnetic arrangement with small magnetic moments was found. The interlayer exchange coupling and the magnetocrystalline anisotropy energy of Fe/V superlattices were studied. The coupling strength was found to vary with the thickness of the iron layers. To describe the in-plane four-fold anisotropy, the inclusion of surface terms proved necessary. The in-plane four fold anisotropy was also studied in a series of Fe/Co superlattices, where the thickness of the Co layers was kept thin so that the bcc structure could be stabilized. Only for samples with a large amount of iron, the easy axis was found to be [100]. The easy axis of bulk bcc Co was therefor suggested to be [111].

This work presents a detailed investigation of magnetization dynamics in synthetic antiferromagnets (SAFs), which has been studied both experimentally, using electrically-detected ferromagnetic resonance (ED-FMR) and vector-network analyzer-based ferromagnetic resonance (VNA-FMR), and theoretically. Two modes, one with in-phase and one with 180° out-of-phase precessing magnetizations of the layers, are identified in all applied field regimes, namely, a low-field antiferromagnetically coupled regime (when magnetizations of the layers have opposite directions), a spin-flop regime at intermediate field values (when magnetizations are non-collinear) and a high-field saturation regime (when both magnetazations are collinear to each other and the external magnetic field direction). The qualitative theoretical description, found to be in good agreement with the experimental data, is given using a system of coupled Landau-Lifshitz equations. In this work, for the first time to our knowledge, it is shown that for SAFs with different magnetic moments of the individual layers, dynamic, and not static, Zeeman and interlayer exchange coupling energies are solely resposible for the frequency-field dependence in the antiferromagnetically coupled regime. The changes in the dynamical energy terms lead to the changes in the dynamical components of the precessing magnetizations. As the external magnetic field is varied, the amplitude of the components vary continiously in different ways for different modes, dropping to zero in the spin-flop regime, which is reflected in the amplitudes of ED-FMR and VNA-FMR. This effect appears only in SAFs with different magnetic moments of the layers and is related to the different increase in the Zeeman energy of the layers as the externally applied field increases. The variation of the dynamical components leads to the modulation of an exchange of spin-angular momentum between the layers (so called spin-pumping effect).This is directly reflected in the measured linewidths for the modes in both ED-FMR and VNA-FMR. As was shown before in the literature and is also confirmed here, spin-pumping leads to a constant difference in linewidths between two modes for SAFs in the saturated case. Here, we extend the previous findings to non-saturated regimes. We show that in non-saturated states, the linewidth difference does not remain constant and varries with the external magnetic field. This linewidth difference changes can be qualitatively explained using the modulation of the dynamical magnetization components. In order to directly model the spin-pumping effects, additional terms are introduced in the coupled Landau-Lifshitz equations, related to the intrinsic damping in the magnetic layers and spin-pumping induced effects. The calculations of linewidth dependences using the extended model are not in full agreement with the experiments, suggesting that additional effects must be added to the model (for example, potential domain formations). Additionly, due to the dependence of the effect on the Zeeman energy asymmetry between the layers of the SAF, SAFs with different ratio of thicknesses are studied. Although the trends described above are common to all the samples, no significant enhancement of spin-pumping effects are observed. Modeling shows that, although the evolution of the dynamical magnetization components does depend on the magnetic moment ratio between the layers, the difference between maximum and minimum values remains almost constant and does not alter the observed linewidth-field dependence.:1 Fundamentals 1 1.1 Magnetic moment 1 1.2 Magnetic energy contributions 6 1.2.1 Zeeman energy 6 1.2.2 Demagnetization energy 7 1.2.3 Magnetic anisotropy 9 1.2.4 Direct Exchange Energy 13 1.2.5 Indirect Exchange. Interlayer Exchange Coupling Energy 15 1.3 Magnetoresistance 17 1.3.1 Ordinary Magnetoresistance 17 1.3.2 Anisotropic Magnetoresistance 20 1.3.3 Giant Magnetoresistance 22 1.4 Magnetization dynamics 25 1.4.1 Classical motivation 25 1.4.2 Quantum mechanical justification 27 1.5 Spin-currents and Spin-pumping 29 2 Experimental methods 33 2.1 Vibrating Sample Magnetometry 33 2.2 Ferromagnetic resonance 34 2.2.1 Cavity-FMR 35 2.2.2 VNA-FMR 36 2.3 Electrically detected ferromagnetic resonance 39 3 Synthetic antiferromagnets. Theoretical model 47 3.1 Static model 47 3.2 Dynamical model 54 4 Sample fabrication and characterization 58 4.1 Fabrication 58 4.2 Static characterization 62 5 Magnetization dynamics in asymmetric SAFs 68 5.1 Dynamical measurements on Py(3nm)/ Ru(0.85 nm)/Py(9 nm) 68 5.2 Theoretical explanation 71 5.3 Dynamics in SAFs with varying asymmetry of the layers 80 6 High-frequency spin-pumping in SAFs 86 6.1 Spin-pumping in magnetic trilayers 86 6.2 Spin-pumping in SAFs 88 6.3 Dependence on the asymmetry between the layers 94 7 Conclusions and outlook 99 A General description of the trilayer system without damping and spin-pumping contributions 102 A.1 Effective fields 103 A.2 Final equations 107 B Mathematica program used for the theoretical modeling 108 B.1 Matrix Elements 108 B.2 Frequency-Modes 109 B.3 Dynamical components and corresponding dynamical energies 112 B.4 Equilibrium condition 114 B.5 Dynamical Energies 118 B.6 Dynamical Trajectories 121 Bibliography 125

Le but de cette thèse est l'étude des propriétés de jonctions tunnel magnétiques à aimantation perpendiculaire, en utilisant l'anisotropie perpendiculaire présente à l'interface entre un métal magnétique et un oxyde. En théorie, dans le cas des applications mémoires, les jonctions tunnel perpendiculaires devraient nécessiter moins d'énergie (courant) pour l'écriture par courant polarisé en spin. Mais la fabrication de telles structures représente un défi et une tâche difficile puisque les propriétés de transport (TMR) et d'anisotropie imposent des contraintes sur les matériaux utilisées en limitant la fenêtre de travail, notamment en ce qui concerne l'épaisseur des couches magnétiques. Pour atteindre cet objectif nous avons tout d'abord étudié les propriétés de ces structures comme l'anisotropie de l'interface métal magnétique-oxyde, le transport tunnel et le couplage entre les couches magnétiques à travers la barrière isolante. L'amplitude de l'anisotropie d'interface entre un métal magnétique et un oxyde dépend de l'épaisseur des couches magnétiques, de la température de recuit et la concentration de l'oxygène à l'interface. Différentes structures ont été réalisées afin de choisir la structure la mieux adaptée pour les applications mémoires MRAM. Une corrélation entre la TMR et l'anisotropie a été observée permettant de valider l'origine de l'anisotropie perpendiculaire : la formation de liaisons métal magnétique-oxygène. Un couplage antiferromagnétique à été aussi observé entre les couches magnétiques à anisotropie perpendiculaire à travers l'oxyde. Une étude détaillée sur le couplage a été faite en fonction de la température de recuit et de l'épaisseur des couches magnétiques pour mieux comprendre l'origine du couplage et une possible relation avec l'amplitude de l'anisotropie perpendiculaire. Finalement des jonctions perpendiculaires ont été nano-lithographiées et des mesures de commutation d'aimantation par transfert de spin sur des piliers nanométriques ont été réalisées avec de faibles courants critiques. / The aim of this thesis is the study of magnetic tunnel junctions with perpendicularly magnetized electrodes (pMTJ), using perpendicular magnetic anisotropy (PMA) arising from the magnetic metal/oxide interfaces. For magnetic memories applications, it was predicted in theory that perpendicular junctions should need less energy (current) for spin transfer torque (STT) writing applications. However, the engineering of such structures is a real challenge and a difficult task since simultaneous transport (TMR) and PMA properties impose constraints on materials being used and also limit the working window of the device, especially in terms of magnetic layer thickness. In order to reach our goal we first studied different properties of these structures, such as the origin of PMA from the metal/oxide interface, tunnel transport and interlayer exchange coupling phenomena. The PMA at magnetic metal/oxide interface was showed to strongly depend on different parameters like annealing temperature, oxygen concentration, layer thickness etc. Several pMTJ structures were tested in order to choose the best one for MRAM memories applications. A correlation between TMR and PMA was observed and confirms the PMA origin from the magnetic metal-oxygen bond formation at the interface. Furthermore, antiferromagnetic interlayer exchange coupling was observed in our structures in the presence of out of plane anisotropy. A detailed study was made as a function of annealing temperature and layers thickness, in order to understand the origin of this coupling and its possible relationship to the anisotropy strength. Finally the STT-pMTJ concept was validated and low critical currents were observed on submicronic dots prepared by electron beam lithography.

Die vorliegende Arbeit befasst sich mit dem ferromagnetischen Kondo-Gitter-Modell (s-d-, s-f-Modell) für Filmstrukturen. Die Spin-Fermion-Wechselwirkung des Modells kommt in Materialien vor, in denen lokalisierte Spins mit beweglichen Ladungsträgern wechselwirken, wie etwa in (verdünnten) magnetischen Halbleitern, Manganaten, oder Seltene-Erd-Verbindungen. Die durch die Ladungsträger vermittelte, indirekte Wechselwirkung zwischen den lokalisierten Spins reicht von der langreichweitigen, oszillierenden RKKY-Austauschwechselwirkung im Falle schwacher Kopplung bis zur kurzreichweitigen Doppelaustausch-Wechselwirkung bei starker Spin-Fermion-Kopplung. Beide Grenzfälle werden in dieser Arbeit durch die Abbildung des Problems auf ein effektives Heisenberg-Modell erfasst. Der Einfluss von reduzierter Translationssymmetrie auf die effektive Austauschwechselwirkung und auf die magnetischen Eigenschaften des ferromagnetischen Kondo-Gitter-Modells wird untersucht. Curie-Temperaturen werden für verschiedene Parameterkonstellationen berechnet. Die Auswirkungen von Ladungstransfer und von Gitter-Relaxation auf die magnetische Oberflächenstabilität werden betrachtet. Die Diskussion bezieht sich auf die Modifizierungen der Zustandsdichte und der kinetischen Energie im dimensionsreduzierten Fall, da die effektiven Austauschintegrale eng mit diesen Größen verknüpft sind. Die Bedeutung von Spinwellen für den Magnetismus dünner Filme und an der Oberfläche wird gezeigt. Die Interlagen-Austauschkopplung stellt ein besonders interessantes und wichtiges Beispiel der indirekten Wechselwirkung zwischen lokalisierten Momenten dar. Im Rahmen einer RKKY-Behandlung wird die Kopplung zwischen Monolagen in dünnen Filmen untersucht. Sie wird entscheidend durch die Art der ebenen und senkrechten Ladungsträgerdispersion bestimmt und ist jenseits eines kritischen Wertes der Fermi-Energie stark unterdrückt. Schließlich wird die temperaturabhängige magnetische Stabilität von interlagen-gekoppelten dünnen Filmen behandelt und die Bedingungen für einen temperaturgetriebenen magnetischen Reorientierungsübergang werden diskutiert. / This thesis is concerned with the ferromagnetic Kondo lattice (s-d, s-f) model for film geometry. The spin-fermion interaction of this model refers to materials in which localized spins interact with mobile charge carriers like in (dilute) magnetic semiconductors, manganites, or rare-earth compounds. The carrier-mediated, indirect interaction between the localized spins comprises the long-range, oscillatory RKKY exchange interaction in the weak-coupling case and the short-range double-exchange interaction for strong spin-fermion coupling. Both limits are recovered in this work by mapping the problem onto an effective Heisenberg model. The influence of reduced translational symmetry on the effective exchange interaction and on the magnetic properties of the ferromagnetic Kondo lattice model is investigated. Curie temperatures are obtained for different parameter constellations. The consequences of charge transfer and of lattice relaxation on the magnetic stability at the surface are considered. Since the effective exchange integrals are closely related to the electronic structure in terms of the density of states and of the kinetic energy, the discussion is based on the modifications of these quantities in the dimensionally-reduced case. The important role of spin waves for thin film and surface magnetism is demonstrated. Interlayer exchange coupling represents a particularly interesting and important manifestation of the indirect interaction among localized magnetic moments. The coupling between monatomic layers in thin films is studied in the framework of an RKKY approach. It is decisively determined by the type of in-plane and perpendicular dispersion of the charge carriers and is strongly suppressed above a critical value of the Fermi energy. Finally, the temperature-dependent magnetic stability of thin interlayer-coupled films is addressed and the conditions for a temperature-driven magnetic reorientation transition are discussed.