Nanomagnetic devices are highly energy efficient and non-volatile. Because of these two attributes, they are potential replacements to many currently used information processing technologies, and they have already been implemented in many different applications. This dissertation covers a study of nanomagnetic devices and their applications in various technologies for information processing – from simulating and analyzing the mechanisms behind the operation of the devices, to experimental investigations encompassing magnetic film growth for device components to nanomagnetic device fabrication and measurement of their performance. Theoretical sections of this dissertation include simulation-based modeling of perpendicular magnetic anisotropy magnetic tunnel junctions (p-MTJ) and low energy barrier nanomagnets (LBM) – both important devices for magnetic device-based information processing. First, we propose and analyze a precessionally switched p-MTJ based memory cell where data is written without any on-chip magnetic field that dissipates energy as low as 7.1 fJ. Next, probabilistic (p-) bits implemented with low energy barrier nanomagnets (LBMs) are also analyzed through simulations, and plots show that the probability curves are not affected much by reasonable variations in either thickness or lateral dimensions of the magnetic layers. Experimental sections of this dissertation comprise device fabrication aspects from the basics of material deposition to the application-based demonstration of an extreme sub-wavelength electromagnetic antenna. Magnetic tunnel junctions for memory cells and low barrier nanomagnets for probabilistic computing, in particular, require ultrathin ferromagnetic layers of uniform thickness, and non-uniform growth or variations in layer thickness can cause failures or other problems. Considerable attention was focused on developing methodologies for uniform thin film growth. Lastly, micro- and nano-fabrication methods are used to build an extreme sub-wavelength electromagnetic antenna implemented with an array of magnetostrictive nanomagnets elastically coupled to a piezoelectric substrate. The 50 pW signal measured from the approximately 250,000-nanomagnet antenna sample was 10 dB above the noise floor.

本論文主要在研究多層膜之垂直異向性結構組成及其介面特質，本實驗多層膜選取的材料為鐵磁性的鈷(Co)以及貴重金屬的鉑(Pt)，並利用濺鍍(Sputtering)系統來製作(鈷/鉑)多層膜樣品，最初的實驗為尋找(鈷/鉑)多層膜結構組成最佳垂直易性發生之條件，所以分別變化鐵磁層鈷之厚度、一般金屬層鉑之厚度、(鈷/鉑)雙層層數及緩衝buffer layer層鉑之厚度，並利用震動樣品磁度儀(VSM)及超導量子干涉儀(SQUIDE)分別量測垂直及平行磁場方向之磁化強度M對磁場field H的關係，再由M-H圖進行判別其垂直異向性的程度。 在最初的實驗部分可了解如何得到最佳(鈷/鉑)垂直異向性多層膜之結構，並從中可得不同緩衝層鉑之厚度、(鈷/鉑)雙層層數及雙層內鉑之厚度的矯頑場有一趨勢存在，於第二部分的實驗即利用這些矯頑場之趨勢來製作一系列產生巨磁效應之三層膜結構，其中的鐵磁層由(鈷/鉑)垂直異向性多層膜取代，並對此結構做一系列量測，利用震動樣品磁度儀(VSM)量測其磁化強度對磁場的關係、利用LR700系統及物理低溫量測系統(PPMS)量測其異常Hall effect霍爾效應(EHE)現象和電阻對磁場的關係，再將這一系列的量測結果分析其中被一般金屬層鉑所隔開的上下(鈷/鉑)垂直異向性多層膜之間耦合程度。 / The topic of this thesis is about the property of the interface and structure in the multilayers with perpendicular anisotropy. The materials of this multilayers are ferromagnetic cobalt and platinum. We use sputtering system to fabricate cobalt/platinum multilayer with various thicknesses. The initial experiment is to search for the optimum condition that develop cobalt/platinum multilayer with perpendicular anisotropy. Then, the influenceof the buffer layer of platinum is studied. We use Vibrating sample magnetometer (VSM) and superconducting quantum interference device (SQUID) magnetometer to measure the magnetization vs. magnetic field relation by applied magnetic fields in both out of plane and in plane directions to distinguishe the degree of perpendicular anisotropy from the M-H figures. From the initial experiments we can understand how to get the optimum structure of cobalt/platinum perpendicular anisotrpy multilayer. There is a tendency exists in the coercivity depending on different thicknesses of the ferromagnetic layer cobalt, the normal noble platinum, the number of bilayers of cobalt/platinum, and the buffer layer of platinum. In the second part of this experiment we used the difference of coercivities to fabricate a series of trilayers structures that produce giant magnetoresistance effect. The individual ferromagnetic layer was cobalt/platinum perpendicular anisotropy multilayer. The structures was measured by VSM to study magnetization vs. field relation. A LR700 resistance bridge and a physical properties measurement system (PPMS) were used to measure the Anomalous Hall Effect (AHE) and resistant vs. field relation.

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.

Le but de la thèse sera d'étudier la faisabilité d'un nouveau procédé de nanostructuration des jonctions tunnel de dimension sub-30nm récemment imaginé et breveté par Spintec et le LTM et de tester les propriétés des jonctions tunnel obtenus sur les plans structural, magnétique et des propriétés électriques. Une attention particulière sera mise sur la caractérisation des défauts générés en bord de piliers lors de la gravure des jonctions tunnels et l'impact de ces défauts sur les propriétés magnétiques et de transport. Une autre partie de la thèse concerne l'optimisation des propriétés magnétiques et de transport des empilements jonctions tunnel magnétiques en vue d'en améliorer la stabilité thermique, l'amplitude de magnétoresistance tunnel et la facilité de gravure de l'empilement.En particulier l'insertion de nouveaux matériaux réfractaires (W, ) dans les empilements a été étudiée pour améliorer la stabilité de l'empilement lors des recuits à haute température. Des améliorations ont également été apportées pour renforcer la stabilité de la couche de référence de la jonction tunnel lorsque cette dernière est située au dessus de la barrière tunnel. Par ailleurs, une nouvelle couche de couplage antiferromagnétique a été mise au point permettant de réduire significativement l'épaisseur totale de l'empilement et par là même facilitant sa gravure.Tous ces résultats ont été obtenus par des mesures magnétiques et de transport réalisées sur les couches continues et sur des piliers de taille nanométriques. / The first aim of the thesis is to study the feasibility of a new process for nanopatterning of sub-30nm diameter tunnel junctions recently patented by Spintec and LTM and to test the properties of tunnel junctions obtained, from the point of view of magnetic and electrical properties. Particular attention will be paid on the characterization of defects generated at the pillar edges when patterning the tunnel junctions and the impact of these defects on the magnetic and transport properties. Another part of the thesis is focused on improving the magnetic and transport MTJ stacks with higher thermal budget tolerance. As a part of this, new materials (W, etc) were used as cap layer or as a spacer layer in composite free layer of pMTJ stacks. Moreover, different magnetic materials combined with different non-magnetic spacer have been investigated to improve the thermal stability factor of the composite storage layers. Detailed structural characterizations were performed to demonstrate the improvements in magnetic and electrical properties. A new RKKY coupling layer was found which allowed to obtain an extremely thin pMTJ stack by reducing the SAF layer thickness to 3.8nm. Seed lees multilayers with enhanced PMA is necesssary to realize a top-pinned pMTJ stack which is necessary to configure a spin-orbit torque MRAM (SOT-MRAM)stack and double magnetic tunnel junction stacks (DMTJs). A new seed less multilyar with enhanced PMA and subsequently advanced stacks such as conventional-DMTJ, thin-DMT, SOT-MRAM stacks, Multibit memory were realized. Finally, electrical properties patterned memory devices were also studied to correlate with the magnetic properties of thin films.

L'amélioration des techniques de dépôts et l’évolution de la compréhension de la physique de la matière condensée a conduit à la découverte de phénomènes nouveaux en électronique de spin (spintronique). En particulier, le retournement de l’aimantation par couple de transfert de spin et couple spin-orbite, ainsi que le développement de dispositifs basés sur la propagation d’ondes de spin ont fait de l’amortissement magnétique de Gilbert un paramètre central pour les futures technologies de stockage et de traitement de l’information. Dans cette étude, la prédiction de valeurs très faibles d’amortissement dans les alliages d’Heusler demi métaux magnétiques Co2MnZ est expérimentalement observée et directement corrélée à la structure électronique sous-jacente. En effet, en substituant l’élément Z dans des couches minces monocristallines de haute qualité de Co2MnZ (Z= Al, Si, Ga, Ge, Sn, Sb) faites par épitaxie par jet moléculaire, les propriétés électroniques telles que le gap de spin minoritaire, la position du niveau de Fermi et la polarisation en spin peuvent être accordées et leurs conséquences sur la dynamique de l’aimantation sont analysées. Les résultats expérimentaux nous permettent de comprendre la relation existante entre la structure électronique mesurée et la valeur d’amortissement magnétique, ainsi que de les comparer aux calculs ab initio. Les valeurs d’amortissement entre 4.1 x10-4 et 9 x10-4 pour Co2MnSi, Co2MnGe, Co2MnSn et Co2MnSb sont les plus petites valeurs jamais reportées pour des couches conductrices et constituent une preuve expérimentale qui confirme les prédictions théoriques sur ces alliages d’Heusler demi métaux magnétiques. Ensuite, la relation entre l’amortissement magnétique de Gilbert et le temps de désaimantation ultra-rapide induit par pulse laser dans la série d’alliages quaternaires Co2MnSixAl1-x à polarisation en spin variable est étudiée. Cette partie vise à vérifier des modèles théoriques qui essaient d’unifier ces deux quantités vivant sur des échelles de temps différentes. Finalement, les propriétés structurales et magnétiques de super réseaux Mn3Ga/Co2YZ sont étudiées dans le but de combiner un amortissement de Gilbert très faible, un gap de spin minoritaire ainsi que l’aimantation perpendiculaire aux plans des couches, une caractéristique indispensable pour des dispositifs à faible consommation d’énergie. / Improvements in thin film elaboration methods and a deeper understanding of condensed matter physics have led to new exciting phenomena in spin electronics (spintronics). In particular, magnetization reversal by spin-orbit and spin-transfer torque as well as the development of spin waves based devices have placed the Gilbert magnetic damping coefficient as a key parameter for future data storage and information processing technologies. The prediction of ultralow magnetic damping in Co2MnZ Heusler half-metal magnets is explored in this study and the damping response is shown to be linked to the underlying electronic structure. By substitution of the Z element in high quality Co2MnZ (Z=Al, Si, Ga, Ge, Sn and Sb) epitaxial thin films grown by molecular beam epitaxy, electronic properties such as the minority-spin band gap, Fermi energy position in the band gap, and spin polarization can be tuned and the consequences for magnetization dynamics analyzed. Experimental results allow us to directly explore the interplay of spin polarization, spin gap and Fermi energy position, with the magnetic damping obtained in these films (together with predictions from ab initio calculations). The ultralow magnetic damping coefficients measured in the range from 4.1 x10-4 to 9 x10-4 for Co2MnSi, Co2MnGe, Co2MnSn and Co2MnSb are the lowest values ever reported in conductive layers and offer a clear experimental demonstration of theoretical predictions on half metal magnetic Heusler compounds. Then, the relation between the Gilbert damping and the ultrafast demagnetization time in quaternary Co2MnSixAl1-x compounds with a tunable spin polarization is analyzed. This way, it is possible to confront theoretical models unifying those two quantities that live in different timescales. Finally, structural and magnetic properties of Mn3Ga/Co2YZ Heusler superlattices are investigated in order to combine ultralow Gilbert damping coefficient, minority spin band gap and perpendicularly magnetized heterostructures, another requirement for low energy consumption devices. Through the present work, we aim to prove that Heusler compounds provide an excellent playground to study fundamental magnetism and offer a pathway for future materials design.

In this thesis multidomain states in magnetically ordered systems with competing long-range and short range interactions are under consideration. In particular, in antiferromagnetically coupled multilayers with perpendicular anisotropy unusual multidomain textures can be stabilized due to a close competition between long-range demagnetization fields and short-range interlayer exchange coupling. These spatially inhomogeneous magnetic textures of regular multidomain configurations and irregular networks of topological defects as well as complex magnetization reversal processes are described in the frame of the phenomenological theory of magnetic domains. Using a modified model of stripe domains it is theoretically shown that the competition between dipolar coupling and antiferromagnetic interlayer exchange coupling causes an instability of ferromagnetically ordered multidomain states and results in three possible ground states: ferromagnetic multidomain state, antiferromagnetic homogeneous and antiferromagnetic multidomain states. The presented theory allows qualitatively to define the area of existence for each of these states depending on geometrical and material parameters of multilayers. In antiferromagnetically coupled superlattices with perpendicular anisotropy an applied magnetic bias field stabilizes specific multidomain states, so-called metamagnetic domains. A phenomenological theory developed in this thesis allows to derive the equilibrium sizes of metamagnetic stripe and bubble domains as functions of the antiferromagnetic exchange, the magnetic bias field, and the geometrical parameters of the multilayer. The magnetic phase diagram includes three different types of metamagnetic domain states, namely multidomains in the surface layer and in internal layers, and also mixed multidomain states may arise. Qualitative and quantitative analysis of step-like magnetization reversal shows a good agreement between the theory and experiment. Analytical equations have been derived for the stray field components of these multidomain states in perpendicular multilayer systems. In particular, closed expressions for stray fields in the case of ferromagnetic and antiferromagnetic stripes are presented. The theoretical approach provides a basis for the analysis of magnetic force microscopy (MFM) images from this class of nanomagnetic systems. Peculiarities of the MFM contrast have been calculated for realistic tip models. These characteristic features in the MFM signals can be employed for the investigations of the different multidomain modes. The methods developed for stripe-like magnetic domains are employed to calculate magnetization processes in twinned microstructures of ferromagnetic shape-memory materials. The remarkable phenomenon of giant magnetic field induced strain transformations in such ferromagnetic shape memory alloys as Ni-Mn-Ga, Ni-Mn-Al, or Fe-Pd arises as an interplay of two physical effects: (i) A martensitic transition creating competing phases, i.e. crystallographic domains or variants, which are crystallographically equivalent but have different orientation. (ii) High uniaxial magnetocrystalline anisotropy that pins the magnetization vectors along certain directions of these martensite variants. Then, an applied magnetic field can drive a microstructural transformation by which the martensitic twins, i.e. the different crystallographic domains, are redistributed in the martensitic state. Within the phenomenological (micromagnetic) theory the equilibrium parameters of multivariant stripe patterns have been derived as functions of the applied field for an extended single-crystalline plate. The calculated magnetic phase diagram allows to give a detailed description of the magnetic field-driven martensitic twin rearrangement in single crystals of magnetic shape-memory alloys. The analysis reveals the crucial role of preformed twins and of the dipolar stray-field energy for the magnetic-field driven transformation process in magnetic shape-memory materials. This work has been done in close collaboration with a group of experimentalists from Institute of Metallic Materials of IFW Dresden, Germany and San Jose Research Center of Hitachi Global Storage Technologies, United States. Comparisons between theoretical and experimental data from this cooperation are presented throughout this thesis as vital part of my work on these different subjects.

Le contexte général de ce travail est le développement et l'intégration de nouveaux matériaux magnétiques ayant des propriétés originales et d'intérêt potentiel pour la spintronique. En tant que matériau ferromagnétique d’aimantation nulle, le composé Sm1-xGdxAl2 (SGA) suscite un intérêt particulier, puisqu’il est capable, dans son état magnétique compensé, de polariser en spin un courant d’électrons. Dans un premier temps, des expériences de photoémission résolues en angle et en spin sur synchrotron ont permis d’effectuer une analyse précise de la structure électronique selon diverses directions de la zone de Brillouin et d’estimer de manière directe la polarisation de spin au niveau de Fermi du composé SGA. Dans un second temps, une attention particulière a été portée aux multicouches [Co/Pt] et aux JTMs à base de [Co/Pt]. Les multicouches [Co/Pt] constituent la seconde électrode des JTMs à base de SGA. Leurs propriétés magnétiques (en particulier l'anisotropie perpendiculaire et l'aimantation à saturation) ont été soigneusement étudiées en fonction de l'épaisseur de Pt et de la nature de la couche tampon (Pt, MgO ou Al2O3), et en liaison avec leurs caractéristiques structurales. Leur intégration dans des JTMs à base de [Co/Pt] a permis ensuite de remonter d’une part à la polarisation tunnel effective des multicouches [Co/Pt] et d’autre part aux configurations magnétiques des différentes électrodes, configurations parfaitement expliquées et reproduites par des simulations micro-magnétiques. Dans un troisième temps, les résultats de magnéto-transport au sein des JTMs SGA/MgO/[Co/Pt] sont présentés et discutés / The general context of this work is the development and integration of new magnetic materials with original properties of potential interest for spintronic applications. In this field, the Sm1-xGdxAl2 (SGA) compound drives a particular attention, as a zero-magnetization ferromagnet that can exhibit a spin polarization in its magnetic compensated state. In a first step, synchrotron-based angle and spin resolved photoemission spectroscopy experiments have permitted to perform an accurate analysis of the electronic structure along various directions of the Brillouin Zone and to get a direct estimation of the spin polarization at the Fermi level. In a second step, a special attention has been the paid to [Co/Pt] multilayers and to [Co/Pt]-based MTJs. The [Co/Pt] multilayers would constitute the second electrode in SGA-based MTJs. Their magnetic properties (especially the perpendicular anisotropy and the saturation magnetization) have been carefully investigated as a function of Pt thickness and nature of the buffer layer (Pt, MgO or Al2O3), and in close connection with structural characteristics. Their integration in [Co/Pt]-based MTJs has permitted to determine the [Co/Pt] effective tunnel polarization and to unravel the magnetic configurations of both electrodes which are perfectly explained and reproduced by micromagnetic simulations. In a third step, the results concerning the magneto-transport experiments in SGA/MgO/[Co/Pt] MTJs are presented and discussed

In this thesis multidomain states in magnetically ordered systems with competing long-range and short range interactions are under consideration. In particular, in antiferromagnetically coupled multilayers with perpendicular anisotropy unusual multidomain textures can be stabilized due to a close competition between long-range demagnetization fields and short-range interlayer exchange coupling. These spatially inhomogeneous magnetic textures of regular multidomain configurations and irregular networks of topological defects as well as complex magnetization reversal processes are described in the frame of the phenomenological theory of magnetic domains. Using a modified model of stripe domains it is theoretically shown that the competition between dipolar coupling and antiferromagnetic interlayer exchange coupling causes an instability of ferromagnetically ordered multidomain states and results in three possible ground states: ferromagnetic multidomain state, antiferromagnetic homogeneous and antiferromagnetic multidomain states. The presented theory allows qualitatively to define the area of existence for each of these states depending on geometrical and material parameters of multilayers. In antiferromagnetically coupled superlattices with perpendicular anisotropy an applied magnetic bias field stabilizes specific multidomain states, so-called metamagnetic domains. A phenomenological theory developed in this thesis allows to derive the equilibrium sizes of metamagnetic stripe and bubble domains as functions of the antiferromagnetic exchange, the magnetic bias field, and the geometrical parameters of the multilayer. The magnetic phase diagram includes three different types of metamagnetic domain states, namely multidomains in the surface layer and in internal layers, and also mixed multidomain states may arise. Qualitative and quantitative analysis of step-like magnetization reversal shows a good agreement between the theory and experiment. Analytical equations have been derived for the stray field components of these multidomain states in perpendicular multilayer systems. In particular, closed expressions for stray fields in the case of ferromagnetic and antiferromagnetic stripes are presented. The theoretical approach provides a basis for the analysis of magnetic force microscopy (MFM) images from this class of nanomagnetic systems. Peculiarities of the MFM contrast have been calculated for realistic tip models. These characteristic features in the MFM signals can be employed for the investigations of the different multidomain modes. The methods developed for stripe-like magnetic domains are employed to calculate magnetization processes in twinned microstructures of ferromagnetic shape-memory materials. The remarkable phenomenon of giant magnetic field induced strain transformations in such ferromagnetic shape memory alloys as Ni-Mn-Ga, Ni-Mn-Al, or Fe-Pd arises as an interplay of two physical effects: (i) A martensitic transition creating competing phases, i.e. crystallographic domains or variants, which are crystallographically equivalent but have different orientation. (ii) High uniaxial magnetocrystalline anisotropy that pins the magnetization vectors along certain directions of these martensite variants. Then, an applied magnetic field can drive a microstructural transformation by which the martensitic twins, i.e. the different crystallographic domains, are redistributed in the martensitic state. Within the phenomenological (micromagnetic) theory the equilibrium parameters of multivariant stripe patterns have been derived as functions of the applied field for an extended single-crystalline plate. The calculated magnetic phase diagram allows to give a detailed description of the magnetic field-driven martensitic twin rearrangement in single crystals of magnetic shape-memory alloys. The analysis reveals the crucial role of preformed twins and of the dipolar stray-field energy for the magnetic-field driven transformation process in magnetic shape-memory materials. This work has been done in close collaboration with a group of experimentalists from Institute of Metallic Materials of IFW Dresden, Germany and San Jose Research Center of Hitachi Global Storage Technologies, United States. Comparisons between theoretical and experimental data from this cooperation are presented throughout this thesis as vital part of my work on these different subjects.