<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.

Magnetic properties of diluted magnetic semiconductors and magnetic metallic multilayers are investigated by SQUID magnetometry. By doping GaAs with magnetic Mn2+ ions under well defined growth conditions, one obtains a diluted magnetic semiconductor, (Ga,Mn)As, in which the randomly-distributed magnetic ions act as acceptor centers. At high enough dopant and hole concentration a carrier-induced ferromagnetic state results between the magnetic ions. Due to peculiarities of the growth process sizable amounts of donor defects, such as Mn interstitials and As antisites, are also introduced into the GaAs host. The magnetic properties of (Ga,Mn)As are altered by the presence of such defects through the compensation effect of the holes. The Mn interstitials are thermally unstable above a certain threshold temperature and therefore their concentration can be controlled by post-growth annealing. The influence of the interfaces on the magnetic moment of FeNi/V and FeNi/Co superlattices has been studied. A decrease of the `FeNi' magnetic moment at the interfaces is observed for FeNi/V superlattices while in case of FeNi/Co an enhanced magnetic moment is obtained at the interfaces. Changes of the interlayer exchange coupling have been studied in a series of Fe/V(Fe) multilayers in which the V spacer was alloyed with small amounts of Fe. The dynamic magnetic properties of discontinuous metal-insulator multilayers of Ni81Fe19/Al2O3 have been investigated. By varying the thickness of the insulator the system exhibits a superferromagnetic, a 3d spin-glass-like and a superparamagnetic behavior.

Phénomènes de spintronique dans les jonctions tunnel magnétiques et des films minces sont très prometteurs des deux points fondamentaux et l'application de vue. Elles sont basées sur l'exploration de spin d'électron en plus de sa charge et comprennent intercalaire couplage d'échange (CEI), l'anisotropie magnétique perpendiculaire (PMA), géante (GMR) et magnétorésistance tunnel (TMR), Couple de transfert de spin (STT), Spin effet Hall (SHE) et même induire du magnétisme dans les éléments non compris d graphène. Cette thèse comprendra premiers principes des études de phénomènes spintronique qui ont été d'un grand intérêt récemment. La première partie est consacrée à intercalaire couplage d'échange à travers les matériaux isolants dont le MgO, SrTiO3, GaAs et ZnSe. La deuxième partie comprendra des études ab initio d'anisotropie magnétique perpendiculaire au Fe | interfaces MgO et MTJ y compris le mécanisme et sa corrélation avec le spin Bloch symétrie Etat fondé de filtrage. Dans les enquêtes troisième partie de l'anisotropie magnétique et la fonction de travail dans les Co | interfaces graphène seront présentés. Ensuite, il sera montré possibilité d'induire et d'optimiser le magnétisme intrinsèque dans nanomeshes graphène. Dernière partie sera consacrée à l'induction de polarisation de spin et le réglage de Dirac point et ordre magnétique dans le graphène à l'aide d'effets de proximité magnétiques substrat. / Spintronic phenomena in magnetic tunnel junctions and thin films are very promising from both fundamental and application points of view. They are based on exploring spin of electron in addition to its charge and include interlayer exchange coupling (IEC), perpendicular magnetic anisotropy (PMA), giant (GMR) and tunnel magnetoresistance (TMR), Spin Transfer Torque (STT), Spin Hall Effect (SHE) and even inducing magnetism in non d elements including graphene. This thesis will include first-principles studies of spintronic phenomena which have been of high interest recently. First part is devoted to interlayer exchange coupling across insulating materials including MgO, SrTiO3, GaAs and ZnSe. The second part will include ab initio studies of perpendicular magnetic anisotropy at Fe|MgO interfaces and MTJs including the mechanism and its correlation to the Bloch state symmetry based spin filtering. In third part investigations of magnetic anisotropy and work function in Co|graphene interfaces will be presented. Next, it will be shown possibility of inducing and optimizing intrinsic magnetism in graphene nanomeshes. Final part will be devoted to inducing spin polarization and tuning Dirac point and magnetic order in graphene by means of magnetic substrate proximity effects.

Dans cette thèse, nous avons étudié la dynamique d'aimantation selon deux échelles de temps en utilisant la technique pompe-sonde magnéto-optique résolue en temps. A l'échelle de la picoseconde, la précession de l'aimantation est induite par des impulsions acoustiques dans des structures multicouches composées de deux couches ferromagnétique séparées par une couche métallique (Ni/Au/Py) avec différentes épaisseurs. La synchronisation de la précession des couches ferromagnétiques couplées a été observée. La modification de la précession de l'aimantation d'une couche de Ni est due l'interaction d'échange intercouche avec la couche Py. A l'échelle de 50fs, nous avons étudié la dynamique magnéto-optique cohérente, athermale, thermale et la relaxation des charges et des spins dans (Ni, Co et Fe) par impulsions de 11 fs dans un régime de faible perturbation. L'interaction spin-orbite et l'interaction d'échange jouent un rôle significatif dans la désaimantation ultrarapide. / In this thesis, we have investigated the magnetization dynamics at picosecond and femtosecond time scale using time resolved magneto-optical pump probe technique. At picosecond time scale, the magnetization precession is induced by ultrafast acoustic pulses in a three layered structure with two ferromagnetic layers separated by varying thickness of metallic spacer layer (Ni/Au/Py). The magnetization precession dynamics of the Ni layer is modified due to the interlayer exchange interaction with the Py layer and the synchronized precession of the coupied ferromagnetic layers has been observed. At the timescale of 50fs, coherent magneto-optical, non-thermal, thermal and relaxation dynamics of charges and spins in ferromagnetic transition metals (Ni, Co and Fe) is studied by using 11fs optical pulses in a very low perturbation regime. The spin orbit interaction and exchange interaction play a significant role in the demagnetization of the ferromagnetic metals induced by femtosecond pulses.

<div>The response time of magnetization switching in current spintronic devices is limited to nanosecond timescales due to the precessional motion of the magnetization during reversal. To overcome this limit two routes of investigation leading to novel recording and logic devices are considered in this thesis: 1) Magnetic tunnel junction structures where the recording and reference layers are replaced by synthetic ferrimagnets and switching is induced by spin transfer torque and 2) Hybrid magneto-photonic devices where switching is induced by plasmon-enhanced all-optical switching. To circumvent limitations of the materials and magnetic properties of CoFeB, the most utilized alloy in spintronics, hcp-CoCrPt, a material that exhibits superior perpendicular anisotropy and thermal stability, is chosen as the ferromagnetic electrode in this work. Whereas actual devices based on the two schemes aforementioned are still in the process of being fabricated, through collaborative work with our international collaborators, this thesis describes fundamental magnetic and structural characterization needed for the realization of said ultrafast switching devices. The magnetic switching behavior of CoCrPt-Ru-CoCrPt synthetic ferrimagnets with perpendicular magnetic anisotropy have been studied in the temperature range from 2K to 300K. It was found that two sets of magnetic transitions occur in the CoCrPt-Ru-CoCrPt ferrimagnet systems studied. The first set exhibits three magnetization states in the 50K – 370K range, whereas the second involves only two states in the 2K and 50K range. The magnetic hysteresis curves of the synthetic ferrimagnet are assessed using an energy diagram technique which accurately describes the competition between interlayer exchange coupling energy, Zeeman energy, and anisotropy energy in the system. This energy diagram analysis is then used to predict the changes in the magnetic hysteresis curves of the synthetic ferrimagnet from 200K to 370K. This represents the potential operation temperature extrema that a synthetic ferrimagnet could be expected to operate at, were it to be utilized as a free layer in a memory or sensor spintronic device in the device configuration described in this dissertation.</div><div>Circularly polarized fs laser pulses generate large opto-magnetic fields in magnetic materials, through the inverse Faraday effect. These fields are attributed to be largely responsible for achieving ultrafast all-optical magnetization switching (AOS). All experimental demonstrations of AOS thus far have been realized on thin films over micron-sized irradiated regions. To achieve magnetization switching speeds in the ps and potentially fs time regimes, this work proposes the use of surface plasmon resonances at the interface of hybrid magneto-photonic heterostructures. In addition to the ability of plasmon resonances to confine light in the nm scale, the resonant excitation can largely enhance induced opto-magnetic fields in perpendicular magnetic anisotropy materials. This requires strong spin-photon coupling between the plasmonic and the magnetic materials, which thus requires the minimization of seed layers used for growth of the magnetic layer. This work reports on the development of ultrathin (1 nm thick) interlayers to control the growth orientation of hcp-Co alloys grown on the refractory plasmonic material, TiN, to align the magnetic axis out-of-plane. CoCrPtTa seed layers down to 1 nm were developed to seed the growth of CoCrPt, and the dependence of the quality of the CoCrPt is investigated as Ta composition is varied in the seed layer. Whereas bismuth iron garnet (BIG) meets the magneto-optical requirements for a hybrid magneto-photonic material, its magnetic and structural properties are highly sensitive to the Bi:Fe ratio and must be grown epitaxially on single crystalline substrates. Therefore, in this work we have investigated alternative materials that offer superior magnetic properties and are amenable to growth on inexpensive substrates. Opto-magnetic field enhancements up to 2.6x in Co-ferrite magneto-photonic heterostructures have been obtained via finite element analysis modelling. Alternative materials for plasmon-enhanced all-optical switching such as Co/Pd multilayers have also been investigated. Successful growth of Co/Pd multilayers on TiN using ultrathin Ti interlayers has been achieved. </div><div><br></div>

Anti-ferromagnetic interlayer exchange coupling between iron layers in Fe/MgO superlatices have recently been of interest among researchers for its potential application in 3D memory storage in computers (hard drives) and in the research field of spintronics. Thinfilms and bi-layers between the 10-100 ångström range in thicknesses were analyzed for its resistive properties during different conditions. Both mono-layers and superlatices were experimented with.The resistivity of the films was measured with both the four-probe method and the Van der Pauw method. Because of mechanical limitations with respect to the direction of the external magnetic field, the Van der Pauw method had to be used for the superlattice measurements. The collected data from all the measurments of the superlattice suggest that the electric current is not only passing the capping layer of the lattice but did not however show any sign of resisitive properties changing with changing magnetic profile. The resistivity of thesuperlattice was similar to that of the resistivity calculated from data when the external magnetic field was off. The results from this study show for the first time that it is possible to measure the electronic transport within an Fe/MgO superlattice which provides a basis for futher investigations.