We have investigated the Faraday effect of bismuth-doped rare-earth iron-garnets with varying doping levels of gallium from z = 1.0 to 1.35. We used lutetium to control the film's in-plane magnetic properties and found that gallium doping levels above the compensation point caused a loss of anisotropy control, a canted out-of-plane magnetization in the film, and an extremely weak but linear coercivity above 10 micro-Tesla fields. Using these results we focused on in-plane films to create 8 layer stacks of 500 um thick films to achieve a minimum detectable field of 50 pT at 1 kHz. Unlike previous Magneto-Optic (MO) studies that typically used thin films of approximately 1um thickness, we used approximately 400um thick films to allow experimentation with the final, robust, ideal form the MO sensor would take. We measured what most other MO studies with garnets neglected: the magnetic anisotropy axis or structure within the film. Knowledge of this structure is essential in improving the sensitivity of a stacked MO probe. Studying thick films proved to be key to understanding the magnetic anisotropy and domain properties that can degrade or enhance the sensitivity of the Faraday rotation in bismuth doped rare-earth iron-garnets to an applied magnetic field and to pointing the direction of future research to develop the conditions for rugged magnetometer sensors. / Physics

Charge transfer at the organic/inorganic semiconductor interfaces lies at the heart of interfacial photochemistry. While decades of research have shaped the current understanding that interfacial charge transfer depends crucially on energetic driving force and electronic coupling, much less is known about the role played by the spin degree of freedom. In particular, it is not clear how spin states evolve during the charge transfer process. With the advent of group 6 transition metal dichalcogenides (TMDC), a class of two-dimensional layered materials which permits the optical generation of spin-polarized electron-hole pairs in the monolayer limit, we now have the opportunity to investigate if charge transfer at an organic/inorganic interface could enable the transfer of spin polarization. Using time-resolved Faraday rotation and transient absorption spectroscopy, it is found in the MoSe₂/H₂Pc and C60/WS₂ heterostructures that the photoinduced hole transfer from MoSe₂ to H₂Pc and electron transfer from WS₂ to C60 results in spin polarization lifetimes one order of magnitude longer than that of a monolayer. In the WS₂/MoSe₂/H₂Pc heterostructure, the addition of a WS₂ monolayer drives the dissociation of electron-hole pairs bound at the MoSe₂/H₂Pc interface and leads to the observation of nanosecond-long spin polarization at room temperature. These findings evidence the photoinduced transfer of spin polarization, a mechanism which could potentially be exploited to enhance the efficiency and selectivity of photochemical reactions involving angular momentum change, and may be generalized to other organic/inorganic interfaces composed of crystalline semiconductors with spin-momentum locking.

Abstract In this thesis nuclear magnetic resonance (NMR) and magneto-optical rotation (MOR) parameters are investigated for water, paying special attention to the effect of solvation from gaseous to liquid phase. Nuclear magnetic shielding and quadrupole coupling tensors of NMR spectroscopy are studied for gaseous and liquid water. Liquid state is modelled by a 32-molecule Car-Parrinello molecular dynamics simulation, followed by property calculations for the central molecules in clusters cut out from the simulation trajectory. Gaseous state is similarly represented by a one-molecule simulation. Gas-to-liquid shifts for shielding constants obtained this way are in good agreement with experiments. To get insight into the local environment and its effect on the properties the clusters are divided into groups of distinct local features, namely the number of hydrogen bonds. The analysis shows in detail how the NMR tensors evolve as the environment changes gradually from the gas to liquid upon increasing the number of hydrogen bonds to the molecule of interest. The study sheds light on the usefulness of NMR experiments in investigating the local coordination of liquid water. To go a bit further, the above mentioned NMR parameters along with the spin-spin coupling constant are examined for water dimer in various geometries to have insight into solvation and hydrogen bonding phenomena from bottom to top. Characteristic changes in the properties are monitored as the geometry of the dimer is systematically varied from very close encounter of the monomers to distances and orientations where hydrogen bonding between monomers ceases to exist. No rapid changes during the hydrogen bond breaking are observed indicating that the hydrogen bonding is a continuous phenomenon rather than an on-off situation. However, for analysis purposes we provide an NMR-based hydrogen bond definition, expressed geometrically, based on the behaviour of the NMR properties as a function of dimer geometry. Our definition closely resembles widely used definitions and thus reinforces their validity. Magneto-optical rotation parameters, the nuclear spin optical rotation (NSOR) and the Verdet constant, are computed for gaseous and liquid water, in the same manner as the NMR properties above. Recent pioneering experiments including NSOR for hydrogen nuclei in liquid water and liquid xenon have demonstrated that this technique has a potential to be a useful new probe of molecular structure. We reproduce computationally, applying a first-principles theory developed recently in the group, the experimental NSOR for hydrogen nuclei in liquid water, and predict hydrogen NSOR in gaseous water along with the oxygen NSOR in liquid and gaseous water. NSOR is an emerging experimental technique that needs interplay between theory and computation for validation, steering and insight.

In this study, the magnetically-induced vibrations of functionalized magnetic particle suspensions were probed for the development of a novel optical spectroscopy technique. Through this work (1) the frequency-dependence of the faraday rotation in ferrofluids and (2) the extension of this system to elucidating particle size and conformation as an alternative immunossay to costly and labor/time intensive Western Blotting and ELISA has been shown. With its sensitivity and specificity, this method has proven to be a promising multi-functional tool in biosensing, diagnostic, and therapeutic nanomedicine efforts. Due to its ubiquitous nature in all optically-transparent materials, the farady rotation, or circular birefringence, was developed as a robust and sensitive nanoscale biomolecule characterization technique through Brownian relaxation studies of particle suspensions. Current efforts have shown the applicability of this phenomenon in solid, pure liquid, and colloidal samples as well as simultaneous advancements of magnetic nanoparticle research in the magnetometric and magneto-optical regimes. By merging these two fields, a clinically relevant spectroscopy (fd-FRS, Frequency Domain Faraday Rotation Spectroscopy) was developed based on a newly revised model stemming from Debye relazation theory. Through this work, an optical bench with a variable permeability core electromagnet and a frequency-domain lock-in amplifier setup (DC to 20 kHz) have been used to distinguish between Fe3O4-core nanoparticles with functionalization layers of PEG4/PEG8 polymer with future applications involving the Anti-BSA/BSA antibody/antigen couple. Particle concentrations down to 500 nM (magnetic nanoparticles) and 0.01 Volume % (magnetic beads) were studied with diameters ranging from 200 nm to 1μm. currently, the characteristic peak corresponding to the out-of-phase relazation of the suspended particles has been elusive, despite a wide particle size distribution and the use of a balanced photodetector. Future work will involved highly monodisperse samples, faster scan times, and thermal characterization applications of fs-FRS.

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

No description available.

Ce travail de thèse est consacré à l’étude des propriétés magnéto-optiques de nanoparticules (NP) magnétiques de ferrite de cobalt (CoFe2O4) sous forme liquide et lorsqu’elles sont bloquées dans une matrice de silice produite par voie sol-gel. Cette dernière dispersion constitue un matériau composite à activité magnéto-optique obtenu par un procédé basse température qui le rend totalement compatible avec les technologies d’intégration. A plus long terme, ce matériau pourra contribuer à l’intégration de composants non-réciproques. L’objectif de ce travail est d’une part l’identification du type de NP qui maximise la rotation Faraday et le facteur de mérite (rapport de la rotation Faraday à l’absorption) dans le but d’améliorer la qualité magnéto-optique du matériau composite. Et d’autre part, il s’agit d’améliorer la compréhension des phénomènes physiques liés aux effets magnéto-optiques de ces nanoparticules et le lien avec leurs caractéristiques physiques. L’étude est menée sur des NP magnétiques synthétisées et dispersées en phase aqueuse au laboratoire PHENIX (UMR CNRS 8234). Les mesures optiques et magnéto-optiques réalisées au laboratoire Hubert Curien (UMR CNRS 5516) ont été complétées par des mesures magnétiques XMCD au synchrotron SOLEIL. L’étude des différentes nanoparticules magnétiques a révélé que l’utilisation d’une petite taille de NP permet de multiplier par deux le facteur de mérite du matériau pour une longueur d’onde de 1,5 µm, soit une division par deux des pertes pour les composants magnéto-optiques visés. L’analyse du comportement spectral de l’effet Faraday illustre l’influence de la distribution cationique des ions Co2+ et Fe3+ dans la structure cristalline. Couplée aux mesures XMCD, l’analyse montre le besoin d’une localisation de l’ion Co2+ en site tétraédrique dans la structure spinelle pour maximiser l’effet Faraday à 1,5µm, et obtenir une anisotropie uniaxe qui permette une pré-orientation aisée des NP lors de la gélification / This work is dedicated to the study of the magneto-optical properties of cobalt ferrite (CoFe2O4) nanoparticles (NP) dispersed in liquid as ferrofluid, or blocked in a solid silica matrix realized with a sol-gel method. This last dispersion is a magneto-optical composite material, obtained with a low temperature process which insures its compatibility with photonic integration technologies, to produce, in the future, integrated non-reciprocal devices. The aim of the study is, on one hand, to identify which kind of NP can improve the Faraday effect and the merit factor (ratio between the Faraday effect and the absorption) of the composite material. On the other hand, the aim is to give a better understanding of the link between the magneto-optical properties and the physical characteristics of the NP. The study has been led on NP synthetized and dispersed as ferrofluid in PHENIX laboratory (UMR CNRS 8234). Optical and magneto-optical measurements were made in Hubert Curien laboratory (UMR CNRS 5516) and completed by XMCD analysis in Synchroton SOLEIL. Results show that it is necessary to use a small size of NP (5 nm) to maximize the merit factor at a wavelength of 1,5 µm. The spectral analysis of the Faraday effect shows the influence of the cationic distribution of Co2+ et Fe3+ in the spinelle structure. Coupled to XMCD results, this analysis shows that it is necessary to maximize the quantity of Co2+ in tetraedric sites to maximize the Faraday effect at 1,5 µm and to obtain an uniaxial anisotropy which allows to orientate the NP during the gelification of the sol-gel matrix

À l'interface entre l'optique, le magnétisme et la supraconductivité, nous cherchons à dévelop-per de nouveaux concepts pour la manipulation optique, la génération et l'étude des vortex d'Abrikosov individuels dans des systèmes supraconducteurs. D'une part, nous démontrons l'efficacité d'une méthode optique de génération spontanée d'une paire de vortex/anti-vortex par effet Kibble Zurek basée sur l'utilisation d'une impulsion laser focalisée à la surface d'un film supraconducteur. C'est une technique en champ lointain, rapide qui permet de créer et piéger une paire dans le condensat supraconducteur à une position stable et reproductible. Cette expérience est également adaptée à l'étude du scénario Kibble-Zurek, relatif à la nucléation spontanée de défauts topologiques, tels que les vortex d'Abrikosov, lors de transitions de phase rapides du second ordre. D'autre part, nous présentons les résultats d'une expérience pompe-sonde visant à étudier l'effet Faraday inverse dans le grenat de BiLuIG servant à l'imagerie magnéto-optique des vortex. Nous montrons qu'il est possible de générer un champ magnétique femtoseconde de plusieurs Tesla localisé dans le grenat grâce à une impulsion laser ultra-courte de polarisation circulaire. Ces résultats nous permettent d'étudier les conditions expérimentales pour une génération de paires de vortex/anti-vortex par méthode magnéto-optique, basée sur l'application d'un fort champ magnétique à la surface du supraconducteur. La possibilité de manipuler et générer les vortex, véritables nano-objets de l'état supraconducteur, offre des perspectives prometteuses quant au développement du contrôle optique de micro-circuits supraconducteurs tels que les jonctions Josephson. / At the interface between optics, magnetism and superconductivity, we want to develop new concepts for the optical manipulation, the generation and the study of individual Abrikosov vortices in superconducting systems. On one hand, we demonstrate the efficiency of an optical method to perform spontaneous generation of a single vortex/anti-vortex pair by Kibble Zurek effect, based on a laser pulse focused at the superconductor film surface. It is a fast far field method to create and trap a pair into the superconducting condensate at a reproducible and stable position. This experiment is also adapted to the study of the Kibble Zurek mechanism, describing nucleation of topological defects such as Abrikosov vortices during a fast second order phase transition. On the other hand, we present the results of a pomp-probe experiment to the study the inverse Faraday effect into a BiLuIG garnet used for magneto-optical imaging of vortices. We show the possibility to produce a strong femtosecond magnetic field of a few Tesla localized into the garnet with a circularly polarized ultra-short laser pulse. Those results lead to the determination of the experimental conditions necessary to generate a vortex/anti-vortex pair with a magneto-optical method based on the application of a strong magnetic field close to the superconductor surface. Fast optical manipulation and generation of vortices, which are intrinsic nano-objects of the superconducting state, should enable the development of optically driven superconducting micro-circuits such as Josephson junctions.

L'essor des télécommunications sur fibres a conduit depuis quarante ans au développement des composants optiques intégrés. Cependant, en raison de difficultés technologiques, un dispositif n'a pas encore été réalisé de façon satisfaisante : il s'agit de l'isolateur optique, dont la fonction est de propager la lumière dans un seul sens. Ces travaux s'inscrivent dans cette problématique puisqu'ils visent à l'intégration d'un isolateur grâce à la technologie de l'échange d'ions Na+/Ag+ sur verre. La configuration adoptée se compose de trois éléments sur puce : un séparateur de polarisation et deux rotateurs de polarisation à 45 °, l'un réciproque et l'autre non. Le séparateur de polarisation a été réalisé sous la forme d'une jonction Y asymétrique. Après une étude théorique, nous présentons le procédé de fabrication ainsi que les résultats expérimentaux obtenus. Les diaphonies mesurées sont à l'état de l'art, elles dépassent (31,1 ± 0,4) dB et (32,7 ± 0,4) dB en mode TE et TM sur une plage spectrale supérieure à 70 nm. Nous avons mené l'étude du rotateur Faraday en collaboration avec le Laboratoire Télécom Claude Chappe de Saint Etienne pour la partie magnéto-optique. La structure employée est un guide d'onde à enterrage différentiel sur lequel est déposé un matériau magnéto-optique par un procédé sol-gel. Un angle de rotation non-réciproque de 50 ° a été mesuré, validant ainsi l'approche hybride. Un nouveau procédé de fabrication est également présenté pour un rotateur réciproque à évolution de mode adiabatique. Celui-ci consiste en un enterrage sous champ présentant une inhomogénéité transverse. Nous proposons finalement une méthode de fabrication de l'isolateur complet basée sur l'intégration monolithique des différents éléments. / For the past forty years, the growth of fiber telecommunications has led to the development of integrated optical components. However, due to technological issues, a device has not yet been realized: the optical isolator, which propagates light in a single direction. Our work fits into this context. It deals with the integration of an isolator using the Na+/Ag+ ion-exchange technology. The configuration we adopted consists of three elements on chip: a polarization splitter and two 45 ° polarization rotators, one is reciprocal and the other is not. The polarization splitter has been realized in the shape of an asymmetrical Y junction. After a theoretical study, we present the fabrication process and experimental results. State-of-the-art diaphonies of (31.1 ± 0.4) dB and (32.7 ± 0.4) dB have been measured in TE and TM mode over a bandwidth larger than 70 nm. The magneto-optical part of the study has been undertaken in collaboration with the Laboratoire Télécom Claude Chappe (LT2C) from Saint Etienne, France. The Faraday rotator is a selectively buried waveguide on which a magneto-optical material has been deposited using a sol-gel process. A non-reciprocal rotation of 50 ° has been measured, hence validating the hybrid approach. A novel fabrication process is presented for a reciprocal mode-evolution polarization rotator. The process consists in the burring of a waveguide under an electric field presenting a transverse inhomogeneity. We finally propose a fabrication method of the complete optical isolator. It is based on the monolithic integration of the three elements.

Abstract In this thesis, the magnetic resonance and magneto-optical rotation parameters are studied in single-layer carbon systems of two different dimensionalities. Based on electronic structure calculations, the spectral parameters are predicted for both extended (2D) and finite, molecular (0D) systems consisting of pure sp²-hybridised pristine graphene (G), as well as hydrogenated and fluorinated, sp³-hybridised graphene derivatives, graphane (HG) and fluorographene (FG), respectively. Nuclear magnetic resonance (NMR) parameters are calculated for G, HG and FG systems at their large-system limit. For their 0D counterparts, graphene flakes, qualitative spectral trends are predicted as functions of their size and perimeter type. The last group of studied carbon systems consists of 2D graphenes containing spin-1/2 paramagnetic defects. Electron spin resonance (ESR) parameters and paramagnetic NMR shieldings are predicted for four different paramagnetic systems, including the vacancy-defected graphane and fluorographene, as well as graphene with hydrogen and fluorine adatoms. The magneto-optic properties of G and HG flakes are studied in terms of Faraday optical rotation and nuclear spin optical rotation parameters, to investigate the effects of their finite size and also the different level of hydrogenation. All the different investigated parameters displayed characteristic sensitivity to the electronic and atomic structure of the studied graphenes. The parameters obtained provide an insight into the physics of these 0D and 2D carbon materials, and encourage experimental verification.