Nanomagnetic devices have been projected as an alternative to transistor-based switching devices due to their non-volatility and potentially superior energy-efficiency. The energy efficiency is enhanced by the use of straintronics which involves the application of a voltage to a piezoelectric layer to generate a strain which is ultimately transferred to an elastically coupled magnetostrictive nanomaget, causing magnetization rotation. The low energy dissipation and non-volatility characteristics make straintronic nanomagnets very attractive for both Boolean and non-Boolean computing applications. There was relatively little research on straintronic switching in devices built with real nanomagnets that invariably have defects and imperfections, or their adaptation to non-Boolean computing, both of which have been studied in this work. Detailed studies of the effects of nanomagnet material fabrication defects and surface roughness variation (found in real nanomagnets) on the switching process and ultimately device performance of those switches have been performed theoretically. The results of these studies place the viability of straintronics logic (Boolean) and/or memory in question. With a view to analog computing and signal processing, analog spin wave based device operation has been evaluated in the presence of defects and it was found that defects impact their performance, which can be a major concern for the spin wave based device community. Additionally, the design challenge for low barrier nanomagnet which is the building block of binary stochastic neurons based probabilistic computing device in case of real nanomagnets has also been investigated. This study also cast some doubt on the efficacy of probabilistic computing devices. Fortunately, there are some non-Boolean applications based on the collective action of array of nanomagnets which are very forgiving of material defects. One example is image processing using dipole coupled nanomagnets which is studied here and it showed promising result for noise correction and edge enhancement of corrupted pixels in an image. Moreover, a single magneto tunnel junction based microwave oscillator was proposed for the first time and theoretical simulations showed that it is capable of better performance compared to traditional microwave oscillators. The experimental part of this work dealt with spin wave modes excited by surface acoustic waves, studied with time resolved magneto optic Kerr effect (TR-MOKE). New hybrid spin wave modes were observed for the first time. An experiment was carried out to emulate simulated annealing in a system of dipole coupled magnetostrictive nanomagnets where strain served as the simulated annealing agent. This was a promising outcome and it is the first demonstration of the hardware variant of simulated annealing of a many body system based on magnetostrictive nanomagnets. Finally, a giant spin Hall effect actuated surface acoustic wave antenna was demonstrated experimentally. This is the first observation of photon to phonon conversion using spin-orbit torque and although the observed conversion efficiency was poor (1%), it opened the pathway for a new acoustic radiator. These studies complement past work done in the area of straintronics.

L’étude présentée dans ce manuscrit s’inscrit dans le domaine du magnétisme de surface, qui a connu de grands développements ces dernières années grâce au microscope à effet tunnel (STM). Elle a pour but de montrer qu’une molécule simple, le nickelocène [Ni(C5H5)2], peut être attachée au sommet d’une pointe STM afin de produire une pointe-sonde magnétique, qui, dans le cadre de l’imagerie magnétique, présente des avantages indéniables comparés à des pointes conventionnelles. À la différence d’autres systèmes moléculaires étudiés avec le STM, nous montrons que les propriétés magnétiques du nickelocène en phase gazeuse sont préservées en présence d’un métal, même lorsque la molécule est attachée au sommet d’une pointe STM. Nous présentons trois résultats marquants avec cette pointe-sonde moléculaire: 1) Nous montrons que l’on peut contrôler le spin du nickelocène, activant à souhait un effet Kondo ; 2) Nous produisons à l’aide du courant tunnel des excitations entre les états de spin du nickelocène, que nous pouvons aisément identifier au travers de la conductance moléculaire. Ces états sont sensibles à toute perturbation magnétique extérieure au nickelocène; 3) Au travers de ces excitations, nous sondons alors le magnétisme de surface. Nous montrons qu’en couplant magnétiquement la pointe-sonde moléculaire avec des atomes, soit isolés soit dans une surface ferromagnétique, nous pouvons mesurer leur polarisation de spin, ainsi que le couplage d’échange nickelocène-atome. Ce dernier permet d’obtenir un contraste magnétique en imagerie STM à l’échelle atomique. / The study presented in this manuscript is part of the field of surface magnetism, which has undergone major developments in recent years thanks to the scanning tunneling microscope (STM). It aims to show that a single molecule, nickelocene [Ni(C5H5)2], can be attached to the tip of a STM to produce a magnetic probe-tip, which, in the context of magnetic imaging, has undeniable advantages compared to conventional tips. Unlike other molecular systems studied with STM, we show that the magnetic properties of nickelocene in the gas phase are preserved in the presence of a metal, even when the molecule is attached to the tip of a STM. We present three remarkable results with this molecular probe-tip: 1) We show that we can control the spin of nickelocene, activating at will a Kondo effect; 2) We monitor the spin states of nickelocene by producing electrically-driven excitations, which we can easily identify through the molecular conductance. These states are sensitive to the magnetic environment surrounding nickelocene; 3) We use these states to probe surface magnetism. We show that by magnetically coupling the molecular probe tip with single atoms, either isolated or in a ferromagnetic surface, we can measure their spin polarization, as well as the nickelocene-atom exchange coupling. By monitoring this coupling it is possible to obtain a magnetic contrast in the STM images with atomic-scale resolution.

In the growing field of spintronics there is a strong need for development of flexible lightweight semi-conducting magnets. Molecular organic-based magnets are attractive candidates since it is possible to tune their properties by organic chemistry, making them so-called “designer magnets”. Vanadium tetracyanoethylene, V(TCNE)x, is particularly interesting since it is a semiconductor with Curie temperature above room temperature (TC~400 K). The main problem with these organic-based magnets is that they are extremely air sensitive. This thesis reports on the frontier electronic structure of the V(TCNE)x by characterization with photoelectron spectroscopy (PES) and near edge x-ray absorption fine structure (NEXAFS) spectroscopy. It also presents a new and more flexible preparation method of this class of organic-based thin film magnets. The result shows improved air stability of the V(TCNE)x prepared with this method as compared to V(TCNE)x prepared by hitherto used methods.

The objective of this dissertation is to classify the opportunities, advantages, and limits of novel interconnects for post-CMOS logic that can augment or eventually replace the CMOS logic. Post-CMOS devices are envisaged on the idea of using state variables other than the electron charge to store and manipulate information. In the first component of the thesis, a comprehensive analysis of the performance and the energy dissipation of novel logic based on various state variables is conducted, and it is demonstrated that the interconnects will continue to be a major challenge even for post-CMOS logic. The second component of the thesis is focused on the analysis of the interconnection aspects of spin-based logic. This research goal is accomplished through the development of physically-based models of spin-transport parameters for various metallic, semiconducting, and graphene nanoribbon interconnects by incorporating the impact of size effects for narrow cross-sectional dimensions of all-spin logic devices. Due to the generic nature of the models, they can be used in the analysis of spin-based devices to study their functionality and performance more accurately. The compact nature of the models allows them to be easily embedded into the developing CAD tools for spintronic logic. These models then provide the foundation for (i) analyzing the spin injection and transport efficiency in an all-spin logic circuit with various interconnect materials, and (ii) estimating the repeater-insertion requirements in all-spin logic, and (iii) estimating the maximum circuit size for all-spin logic. The research is crucial in pinpointing the implications of the physical limits of novel interconnects at the material, device, circuit, and architecture levels.

<p>In the growing field of spintronics there is a strong need for development of flexible lightweight semi-conducting magnets. Molecular organic-based magnets are attractive candidates since it is possible to tune their properties by organic chemistry, making them so-called “designer magnets”. Vanadium tetracyanoethylene, V(TCNE)_x, is particularly interesting since it is a semiconductor with Curie temperature above room temperature (T_C~400 K). The main problem with these organic-based magnets is that they are extremely air sensitive. This thesis reports on the frontier electronic structure of the V(TCNE)_x by characterization with photoelectron spectroscopy (PES) and near edge x-ray absorption fine structure (NEXAFS) spectroscopy. It also presents a new and more flexible preparation method of this class of organic-based thin film magnets. The result shows improved air stability of the V(TCNE)_x prepared with this method as compared to V(TCNE)_x prepared by hitherto used methods.</p>

Nous étudions plusieurs problémes reliés aux propriétés de transport dans les systèmes corrélés. La thèse contient 3 parties distinctes, chacune d'entre elles décrivant un aspect particulier. Nous avons obtenu dans chacun des cas des résultats qui permettent une meilleure compréhension du transport. Nous étudions l'effet de la dissipation et d'une perturbation extérieure dépendant du temps sur le diagramme de phases d'un systèmes à N corps à température nulle et à température finie. En présence de perturbation dépendant du temps, la dissipation joue un rôle important dans l'évolution vers un état stable indépendant du temps. Nous utilisons le formalisme de Keldysh dans l'approximation adiabatique qui permet d'étudier le diagramme de phases du système en fonction de parameter et de la température. Dans la 2ième partie, nous étudions un concept important pour la physique des systèmes métalliques à plusieurs bandes, le concept d'hybridation, et la façon dont l'hybridation affecte la supraconductivité du métal. De façon générale, une hybridation dépendante ou non du vecteur d'onde k a tendance à détruire la supraconductivité. Nous montrons dans ce chapitre qu'une hybridation antisymétrique a l'effet inverse et renforce la supraconductivité. Nous montrons que si l'hybridation est antisymétrique, la supraconductivité a des propriétés non-triviales. Nous proposons que dans un tel système, il puisse exister des fermions de Majorana, même en l'absence de couplage spin-orbite. Le dernier chapitre de la thèse porte sur les effets du couplage spin-orbite sur le transport dans les nanostructures magnétiques. Dans les nanostructures, le couplage spin-orbite joue un rôle important en raison de la brisure de symmétrie à la surface ou aux interfaces. En particulier, nous étudions l'effet de l'interaction Dzyaloshinskii-Moriya (DM) sur le transport de spin dans un système tri-couche. Nous montrons qu'il existe une interaction DM entre les moments des couches et les électrons de conduction, et l'influence de cette interaction sur le transport est étudiée dans un modèle simplifié ou chaque couche est représentée par un point. / We study some important problems related to the transport properties of many body systems. It is divided in three parts, each one focusing in a specific topic. We obtain relevant results that improve our understanding of these systems. We investigate the effect of dissipation and time-dependent external sources, in the phase diagram of a many body system at zero and finite temperature. In the presence of time-dependent perturbations, dissipation is essential for the system to attain a steady, time independent state. In order to treat this time dependent problem, we use a Keldysh approach within an adiabatic approximation that allows us to study the phase diagram of this system as a function of the parameters of the system and temperature. We also discuss the nature of the quantum phase transitions of the system. Next, we study an important concept in the physics of metallic multi-band systems, that of hybridization, and how it affects the superconducting properties of a material. A constant or symmetric $k$-dependent hybridization in general act in detriment of superconductivity. We show here that when hybridization between orbitals in different sites assumes an anti-symmetric character having odd-parity it {it{enhances}} superconductivity. The antisymmetric hybridization in a problem study in this thesis (present in Chapter 3) allow us to propose a new system where it is possible to investigate Majorana fermions, even in absence of spin-orbit interactions. In the last part of this thesis we study the effect of spin-orbit coupling (SOC) on transport properties in magnetic nanostructures. In this system SOC plays an important role, because surfaces (or interfaces) introduce symmetry breaking which is a source of spin-orbit interaction. We study the role of Dzyaloshinshkii-Moriya (DM) interaction on spin-transport in a 3 layer system. We show that there is a DM interaction between magnetics ions in the layers and spin of conduction electrons. We study the influence of this DM interaction on transport within a simple model where each layer is represented by a point.

A system with two magnetic molecules embedded in a junction between non-magnetic leads was studied. In this system electrons tunnel from the localized energy level in region one to the localized energy level in region two generating a flow of electric charge through the quantum dot system. The current density and thus the conductance changes depending on the molecular spin moment. In this work we studied molecules with either spin "up" or spin "down" and with symmetric coupling strengths. The results indicate that the coupling strength between energy level and molecule together with the tunneling rate through the insulating layer play a major role when switching from parallel to anti-parallel molecular spin, for a specific combination of the coupling strength and tunneling rate we could observe a decrease in the current by 99.7% in the non-gated system and 99.4% in the gated system.

This thesis is centred around the study materials with novel electronic properties, including transition metals interacting with semiconductors and unique molecular systems. The idea of advancing modern computing is the basis for motivating the work in that the projects all have potential to be used in novel applications that would impact the efficiency and/or execution of current technology. We have studied two variations of transition metals as they appear in materials and two molecular systems. As for the transition metals interacting with semiconductors, we first discuss transition metal atoms introduced as impurities to a semiconductor lattice, and second, we discuss transition metal oxides that are naturally semiconducting. We have used a number of experimental and theoretical techniques to better understand these groups of materials. Materials prepared through high quality synthesis techniques were studied using x-ray spectroscopy made possible by synchrotron light sources. Computational software then allowed for the experiments to be interpreted by comparing them to the simulations. In the study of transition metals as impurities, we chose the Co:MoS2 system because MoS2 has had promising results with other transition metal dopants. We examined the electronic structure for two purposes: (1) to determine the local bonding environment and locations of the cobalt atoms in order to better understand the behaviour of Co as an impurity; and (2) the overall band gap of the system so that we could evaluate the system’s potential for use in applications. Experimental results combined with our theoretical simulations led us to conclude that the samples available were all metallic, and at low concentrations cobalt atoms were able to substitute directly into the MoS2 lattice. An examination of copper (II) oxide allowed us to investigate the ability to tune the band gap of a known semiconductor through a synthesis process that applied axial pressure to the sample. For a collection of samples prepared at different pressures, x-ray spectroscopy methods showed an increasing band gap with increasing synthesis pressure, a result that is most encouraging for the field of band gap engineering. Using soft x-ray spectroscopy to examine the conduction and valence bands of the two molecular systems, the potassium-doped hydrocarbons and Li2RuO3, was important for drawing conclusions about the materials’ composition and behaviour. Results showed the introduction of new states at the lower edge of the conduction band of K:phenanthrene, a possible reason for its low-temperature superconductivity. Li2RuO3’s electronic structure was examined and compared to calculations performed by collaborators.

Two of the principal phenomena observed and exploited in the field of spintronics are giant magnetoresistance (GMR) and spin transfer torque (STT). With GMR, the resistance of a magnetic multilayer is affected by the relative orientation of its magnetic layers due to (electron) spin dependent scattering. For the STT effect, a spin-polarized electric current is used to alter the magnetic state of a ferromagnet. Together, GMR and STT are at the foundation of numerous technologies, and they hold promise for many more applications. To achieve the high current densities (~10¹² A/m²) that are necessary to observe STT effects, point contacts – constricted electrical pathways (~1–100 nm in diameter) between conducting materials – are often used because of their small cross-sectional areas. In this sense, we have explored STT in bilayer magnetic nanopillars, where an electric current was used to induce precession of a ferromagnetic layer. This precessional state was detected as an increase in resistance of the device, akin to GMR. Temperature dependent measurements of the onset of precession shed light on the activation mechanism, but raised further questions about its detailed theory. Point contacts can also be used as local sources or detectors of electrons. In this context, we have observed transverse electron focusing (TEF) in a single crystal of bismuth. TEF is a k-selective technique for studying electron scattering from within materials. Using lithographically fabricated point contacts, we have studied the temperature dependence of the relaxation time for ballistic electrons from 4.2 to 100 K. These measurements indicated a transition between electron-electron dominated scattering at low temperatures and electron-phonon scattering as the Debye temperature was approached. We present preliminary work toward a TEF experiment to measure spin dependent scattering from a non-magnet/magnet interface. We also investigated spin wave propagation in thin, magnetic waveguide structures. At the boundary between the waveguide and continuous magnetic film, spin wave rays were found to radiate into the film, or to reflect and form standing waves in the waveguide. A circular defect in the waveguide was observed to cause diffraction of spin waves, generating an interference pattern of higher modes of oscillation. / text

In the last years, the progressive miniaturization of magnetic storage devices has imposed the necessity to understand how the physical properties are modi- ed with respect to the bulk when the dimensions are reduced at the nanometric scale. For this reason an accurate method of preparation and characterization of nanostructures is extremely important. This work focuses on the magnetic and transport properties of cluster-assembled nanostructures, namely cobalt nanoparticles embedded in copper matrices. Our setup allows us to independently control the mean cluster size, the concentration and the chemical composition. The cobalt cluster production is based on magnetron sputtering and gas phase aggregation. The performance of the source permits a wide range of cluster masses, from one to several thousand atoms. As a rst step we studied the role of inter-particle interactions in the transport and magnetic properties, increasing the cobalt nanoparticle concentration (from 0.5% to 2.5% and 5%). Our results demonstrate the necessary precautions and constitute a solid basis for further studies of the spintronic properties of granular systems. Finally, in order to describe the intrinsic magnetic properties of cluster-assembled nanostructures, we prepared strongly diluted samples (<0.5%) for di erent cluster sizes from 1.9 nm to 5.5 nm. We found that the magnetic properties are size-dependent. Using a complete magnetic characterization, sensitive to the change in the e ective magnetic anisotropy, we show that the magnetic anisotropy is dominated by the contributions of the surface or of the shape of the nanoparticles.