Le projet de thèse est divisé en deux parties. D’une part, la génération directionnelle et singulière de plasmons de surface (SPPs) par des ouvertures nanométriques a été réalisé et optimisé par le biais de microscopie de fuites radiatives (LRM). Nous démontrons expéri- mentalement qu’une structure plasmonique composée de nano-ouvertures en forme de T et Λ permet de contrôler le couplage unidirectionnel et radialdes SPPs grâce au spin de la lumière incidente. Pour confirmer nos résultats expérimentaux, nous développons un modèle analytique qui décrit les coupleurs plasmoniques constitués de nano-ouvertures par représentation multidipolaire, permettant ainsi une explication théorique de la directionalité et de la formation de vortex plasmonique. L’optimisation des paramètres géométriques tels que l’angle au sommet des ouvertures en forme de Λ montre la possibilité de maximiser la directivité et le taux d’extinction à la fois pour le couplage directionnel et la génération des vortex dans le champ lointain. Parailleurs, notre méthode basée sur la détection LRM, permet une analyse quantitative et est avérée être une technique de caractérisation sophistiquée pour cartographier le champ plasmonique. Il fournit également plusieurs nouvelles possibilités pour la focalisation de SPP contrôlée en polarisation.D’autre part,le couplage spin-orbite de la lumière dans un guide et son effet réciproque sont réalisées et confirmées expérimentalement et théoriquement. Les coupleurs et découpleurs réseaux sur le guide d’ondes sont d’abord développés et étudiés. La sortie parfaite de la lumière confinée par le découpleur nous offre la possibilité de détecter les ondes guidées. La fluorescence des nanocristaux déposés sur la surface de l’échantillon montre une autre possibilité de visualiser directement la propagation de la lumière dans le guide d’onde. Le couplage directionnel contrôlé par spin est réalisé par des antennes en forme de Λ et est confirmé par des images en champ sombre avec des découpleurs et des images de fluorescence. En outre, l’effet réciproque est observé avec une imperfection de polarisation de sortie qui est expliqué théoriquement par le fait que les ordres de diffraction par les antennes en forme de Λ influent sur les états de polarisation finaux. Ainsi, l’effet réciproque est parfaitement réalisé par la sélection d’une région spécifique de diffraction dans le plan de Fourier. La caractérisation quantitative des interactions spin-orbite nous permet d’envisager le développement de nouveaux coupleurs directionnels dans le domaine de la nanophotonique tels que le traitement quantique de l’information. / In this project, two contributions are reported. Firstly, the directional and singular generation of Surface Plasmon Polaritons (SPPs) in the nanoapertures is investigated using the Leakage Radiation Microscopy (LRM). We demonstrate experimentally spin-driven directional coupling as well as singularity (inward) and vortex (outward radial coupling) of SPPs by nanostructures built with T-shaped and Λ-shaped apertures.To support our experimental findings, we develop an analytical model based on a multidipolar representation of Λ- andT-shaped aperture plasmonic couplers, allowing a theoretical explanation of both directionality and singular SPP formation. The optimal apex angle of Λ-shaped apertures shows the possibility to maximize the directiviy and extinction ratio for both directional coupling and singular SPP generation in the far field. Besides, our method based on LRM detection, allows quantitative analysis and is proven to be a sophisticated characterization technique for mapping the SPP vortex field.It also provides several new possibilities for polarization-controlled SPP sub-wavelength focusing.Secondly, the spin-orbit coupling of light into a photonic waveguide and its reciprocal effect are realized and confirmed both experimentally and theoretically. Coupler and decoupler gratings on the waveguide are firstly developed and investigated. The radiation of the confined light from the decoupler provides us a possibility to detect the guided waves. The fluorescence of nanocrystals deposited on the sample surface shows another possibility to directly visualize the light propagation in the waveguide. The spin-driven directional coupling is achieved by Λ-shaped antennas and is certified by the dark field images with decouplers and the fluorescence images. Furthermore, the reverse effect is observed with an imperfection of output polarization which is explained that the diffraction orders by the Λ-shaped apertures influence the final polarization states based on an analytical model. Thus, the reciprocal effect is realized by selecting the specific diffraction region on the Fourier plane. We believe that the quantitative characterization of spin-orbit interactions will pave the way for developing new directional couplers in the field of nanophotonics such as quantum information processing and so forth.

The layered iridates such as Sr2IrO4 and Sr3Ir2O7, have attracted substantial attention due to their novel electronic states originating from strong spin-orbit coupling and electron-correlation. Recent studies have revealed the possibilities of novel phases such as topological insulators, Weyl semimetals, and even a potential high-Tc superconducting state with a d-wave gap. However, there are still controversial issues regarding the fundamental electronic structure of these systems: the origin of the insulating gap is disputed as arising either from an antiferromagnetic ordering, i.e. Slater scheme or electron-correlation, i.e. Mott scheme. Moreover, it is a formidable task to unveil the physics of layered iridates due to the limited number of available materials for experimental characterizations. One way to overcome this limit and extend our investigation of the layered iridates is using metastable materials. These materials which are far from their equilibrium state, often have mechanical, electronic, and magnetic properties that different from their thermodynamically stable phases. However, these materials cannot be synthesized using thermodynamic equilibrium processes. One way to synthesize these materials is by using pulsed laser deposition (PLD). PLD is able to generate nonequilibrium material phases through the use of substrate strain and deposition conditions. Using this method, we have synthesized several thermodynamically metastable iridate thin-films and have investigated their electronic and optical properties. Synthesizing and investigating metastable iridates opens a path to expand the tunability further than the ability of the bulk methods. This thesis consists of four studies on metastable layered iridate thin film systems. In the first study, three-dimensional Mott variable-range hopping transport with decreased characteristic temperatures under lattice strain or isovalent doping has been observed in Sr2IrO4 thin films. Application of lattice strain or isovalent doping exerts metastable chemical pressure in the compounds, which changes both the bandwidth and electronic hopping. The variation of the characteristic temperature under lattice strain or isovalent doping implies that the density of states near the Fermi energy is reconstructed. The increased density of states in the Sr2IrO4 thin films with strain and isovalent doping could facilitate a condition to induce unprecedented electronic properties, opening a way for electronic device applications. In the second study, the effects of tuning the bandwidth via chemical pressure (i.e., Ca and Ba doping) on the optical properties of Sr2IrO4 epitaxial thin films has been investigated. Substitution of Sr by Ca and Ba ions exerts metastable chemical pressure in the system, which changes both the bandwidth and electronic hopping. The optical conductivity results of these thin films suggest that the two-peak-like optical conductivity spectra of the layered iridates originates from the overlap between the optically-forbidden spin-orbit exciton and the inter-site optical transitions within the Jeff = ½ band, which is consistent with the results obtained from a multi-orbital Hubbard model calculation. In the third study, thermodynamically metastable Ca2IrO4 thin- films have been synthesized. Since the perovskite structure of Ca2IrO4 is not thermodynamically stable, its bulk crystals do not exist in nature. We have synthesized the layered perovskite phase Ca2IrO4 thin- films from a polycrystalline hexagonal bulk crystal using an epitaxial stabilization technique. The smaller A-site in this compound compared to Sr2IrO4 and Ba2IrO4, increases the octahedral rotation and tilting, which enhance electron-correlation. The enhanced electron-correlation is consistent with the observation of increased gap energy in this compound. This study suggest that the epitaxial stabilization of metastable-phase thin-films can be used effectively for investigating complex-oxide systems. Finally, structural, transport, and optical properties of tensile strained (Sr1-xLax)3Ir2O7 (x = 0, 0.025, 0.05) thin-films have been investigated. While high-Tc superconductivity is predicted in the system, all of the samples are insulating. The insulating behavior of the La-doped Sr3Ir2O7 thin-films is presumably due to disorder-induced localization and ineffective electron-doping of La, which brings to light the intriguing difference between epitaxial thin films and bulk single crystals of the iridates. These studies thoroughly investigate a wide array of novel electronic and optical phenomena via tuning the relative strengths of electron correlation, electronic bandwidth, and spin-orbit coupling using perturbations such as chemical doping, and the stabilization of metastable phases in the layered iridates.

<b>Résumé:</b> Dans le but de décrire la rotation résonante rigide de Mercure, différents modèles de rotation résonante de type 3 : 2 à deux et trois dimensions, moyennisés sur les courtes périodes et exprimés en formalisme hamiltonien sont proposés. Dans le premier modèle, l'axe de rotation de Mercure est confondu avec son plus petit axe d'inertie et la planète n'est soumise à l'action d'aucune force autre que celle de la gravitation. Le couplage de ces 2 degrés de liberté est mis en évidence. Un modèle à 3 degrés de liberté tenant compte de la dissociation de l'axe du moment angulaire et de l'axe de figure est ensuite présenté. Dans ces deux modèles, le développement du potentiel est limité à l'ordre 2 en excentricité. Afin d'estimer l'erreur commise par ce choix de troncature, les Hamiltoniens sont développés à des ordres plus élevés; les nouveaux termes ainsi obtenus sont considérés comme des perturbations et traités à l'aide de la théorie de Lie. L'influence des autres planètes du Système Solaire est enfin étudiée en incluant, dans un premier temps, une précession constante du noeud ascendant et du péricentre dans notre modèle de base et, dans un second temps, en considérant que l'inclinaison et l'excentricité sont des fonctions lentes du temps permettant l'utilisation de la théorie de l'invariant adiabatique étendue à 2 degrés de liberté. Une étude des équilibres et des périodes propres de chaque modèle est réalisée.// <b>Abstract:</b> In the aim to describe the Mercury's rigid resonant rotation, different 3: 2 spin-orbit resonant rotation models with two and three dimensions , averaged on the short periods and expressed in Hamiltonian formalism is proposed. In the first model, Mercury's rotation axis and its smallest axis of inertia aren't distinct and no force except the gravitation one acts on the planet. The coupling between these 2 degrees of freedom is underlined. A 3 degrees of freedom model taking into account the dissociation of the angular momentum axis from the figure axis is aftewards presented. In these two models, the potential devellopment is limited to the second order in eccentricity. In order to estimate the error due to this troncature choice, the Hamiltonians are devellopped up to higher orders; the new terms so obtained are considered as perturbations et treated thanks to Lie theory. The influence of the other planets of the Solar System is finally studied by including, in a first time, a constant precession of the ascending node and of the pericenter in our basis model and, in a second time, by considering that the inclination and the excentricity are slow functions of time allowing the use of the adiabatique invariant extended to 2 degrees of freedom. A study of the equilibria and of the proper periods of each model is realized.

The underlying theory of “Spin” of an electron and its associated inter-actions causing internal fields and spectral shift to bulk-magnetism iswell established now. Our understanding of spin properties is significant andmore useful than ever before. In recent years there seems to be an enormousinterest towards application oriented materials that harness those spin prop-erties. Theoretical simulations remain in a position to “assist or pilot” theexperimental discovery of new materials.In this work, we have outlined available methodologies for spin coupling inmulti-reference and DFT techniques. We have benchmarked multi-referencespin-Hamiltonian computation in isoelectronic diradicals - Trimethylenemethane(TMM) and Oxyallyl. Also with DFT, parameters are predicted with anewly discovered TMM-like stable diradicals, reported to have large positiveexchange interactions. Excellent agreement were obtained and our findingsemphasize that the dipole-dipole interactions alone can predict the splittingof triplet states and that DFT spin procedures hold well in organic species.We have extended our spin-studies to a highly application oriented ma-terial - nanographene. Using our novel spin-parameter arguments we haveexplained the magnetism of graphene. Our studies highlight a few signifi-cant aspects - first there seems to be a size dependency with respect to thespin-Hamiltonian; second, there is a negligible contribution of spin-orbit cou-pling in these systems; third, we give a theoretical account of spin restrictedand unrestricted schemes for the DFT method and their consequences forthe spin and spatial symmetry of the molecules; and, finally, we highlightthe importance of impurities and defects for magnetism in graphene. Wepredict triplet-singlet transitions through linear response TDDFT for thetris(8-hydroxyquinoline) aluminium complex, an organic molecule shown tohave spintronics applications in recent experiments. Our spin studies werein line with those observations and could help to understand the role of thespin-coupling phenomena. / QC 20120531

No description available.

There is no apparent, dominant interaction in heavy transition metal oxides (TMO), especially in 5d-TMO, where all relevant interactions are of comparable energy scales, and therefore strongly compete. In particular, the spin-orbit interaction (SOI) strongly competes with the electron-lattice and on-site Coulomb interaction (U). Therefore, any tool that allows one to tune the relative strengths of SOI and U is expected to offer an opportunity for the discovery and study of novel materials. BaIrO3 is a magnetic insulator driven by SOI whereas the isostructural BaRuO3 is a paramagnetic metal. The contrasting ground states have been shown to result from the critical role of the strong SOI in the iridate. This dissertation thoroughly examines a wide array of newly observed novel phenomena induced by adjusting the relative strengths of SOI and U via a systematic chemical substitution of the Ru4+(4d4) ions for Ir4+(5d5) ions in BaIrO3, i.e., in high quality single crystals of BaIr1-xRuxO3(0.0 < x < 1.0) . Our investigation of structural, magnetic, transport and thermal properties reveals that Ru substitution directly rebalances the competing energies so profoundly that it generates a rich phase diagram for BaIr1-xRuxO3 featuring two major effects: (1) Light Ru doping (0 < x < 0.15) prompts a simultaneous and precipitous drop in both the magnetic ordering temperature TC and the electrical resistivity, which exhibits metal-insulator transition at around TC. (2) Heavier Ru doping (0.41 < x < 0.82) induces a robust metallic and spin frustration state. For comparison and contrast, we also substituted Rh4+(4d5) ions for Ir4+(5d5) ions in BaIrO3, i.e. BaIr1-xRhxO3(0.0 < x < 0.10), where Rh only reduces the SOI, but without altering the band filling. Hence, this system remains tuned at the Mott instability and is very susceptible to disorder scattering which gives rise to Anderson localization.

No description available.

Cette thèse porte sur l'étude d'oxydes d'iridium dont le fort couplage spin-orbite est susceptible de générer de nouvelles phases électroniques et magnétiques. Deux familles de composés ont été considérées: Sr3MM’O6, à chaines de spins mixtes arrangées sur réseau triangulaire, et R2Ir2O7, à réseaux pyrochlores interpénétrés de spins. Ils ont été synthétisés sous forme polycristalline et pour certains sous forme monocristalline puis étudiés macroscopiquement par mesure d'aimantation. Ils ont ensuite été sondés microscopiquement par diffusion de neutrons et de rayons X. Nos mesures montrent que dans les composés à chaînes de spins Sr3NiPtO6 et Sr3NiIrO6 les ions Ni2+ présentent une très forte anisotropie magnétocristalline planaire perpendiculaire à l'axe des chaînes. Nous démontrons que ceci stabilise dans Sr3NiPtO6 une phase non magnétique dite « large-D ». Cette anisotropie se manifeste dans Sr3NiIrO6 à haute température. Ce composé s'ordonne cependant à basse température dans une structure magnétique avec les moments alignés le long de l'axe des chaînes. Nous expliquons ce changement d'anisotropie comme étant dû à la présence des ions Ir4+ dont le couplage spin-orbite produit une forte anisotropie des interactions Ni-Ir qui confinent les moments magnétiques le long des chaînes. Concernant les pyrochlores iridates R2Ir2O7, les mesures d'aimantation et de diffraction de neutron sont cohérents avec un ordre "all-in/all-out" des moments magnétiques des ions Ir4+, révélé indirectement via le comportement du sous-réseau des terres rares R. Cet ordre est le seul compatible avec la phase semi-métal de Weyl prédite comme résultant du fort couplage spin-orbite. Le comportement du sous-réseau de terre rare R dépend de l'anisotropie magnétocrystalline des ions R3+. Les ions à anisotropie uniaxiale locale sont polarisés par le champ moléculaire produit par l'ordre de l'iridium dont la direction coïncide avec l'axe d'anisotropie. Les ions à anisotropie locale planaire perpendiculaire à cette direction ne présentent pas d’ordre magnétique induit par celui de l'iridium. A plus basse température, les interactions entre terres rares génèrent des comportements magnétiques plus complexes. / This thesis focuses on the study of iridium oxides, in particular on the consequences of the strong spin-orbit coupling of the iridium. Two families of compounds have been investigated: Sr3MM’O6, with mixed spin chains arranged on a triangular lattice, and R2Ir2O7 with interpenetrated pyrochlores networks of spins. Polycrystalline samples have been synthetized and in some instances single crystals were successfully grown. They were investigated macroscopically by magnetization measurements and probed microscopically by neutron and synchrotoron X-ray scattering experiments. Our measurements showed that in the spin chain compounds Sr3NiPtO6 and Sr3NiIrO6 the Ni2+ ions show a strong easy plane magnetocrystalline anisotropy, perpendicular to the chain axis. This stabilizes in Sr3NiPtO6 the so-called "large-D" non-magnetic phase. The planar anisotropy comes out in Sr3NiIrO6 at high temperature. The compound however orders at low temperature in a magnetic configuration with all the magnetic moments confined along the chain axis. We explain this change of anisotropy as due to the Ir4+ ions whose spin-orbit coupling produces a strong anisotropy of the intra-chain Ni-Ir magnetic interactions overwhelming the single-ion Ni2+ anisotropy. Concerning the pyrochlore iridates R2Ir2O7, magnetization measurements and neutron powder diffraction experiments are consistent with an "all-in/all-out" magnetic ordering of the Ir magnetic moments, revealed indirectly through the magnetic behavior of the rare-earth sublattice. This ordering is the only one consistent with a Weyl semi-metal phase predicted to arise from the spin-orbit coupling. The magnetic behavior of the rare-earth sublattice depends on the rare earth magnetocrystalline anisotropy. The ions with local uniaxial anisotropy are polarized by the Ir molecular field, whose direction coincides with the anisotropy axis. The ions with local planar anisotropy perpendicular to this direction show no iridium induced long-range magnetic ordering. At lower temperature, rare-earth interactions generate more complex magnetic behaviors.

xv, 215 p. : ill. (some col.) A print copy of this thesis is available through the UO Libraries. Search the library catalog for the location and call number. / In this dissertation, several new methods for the measurement and control of transverse photonic degrees of freedom are developed. We demonstrate a mode sorter for two-dimensional (2-D) parity of transverse spatial states of light based on an out-of-plane Sagnac interferometer. The first experimental 2-D parity sorting measurements of Hermite-Gauss transverse spatial modes are presented. Due to the inherent phase stability of this type of interferometer, it provides a promising tool for the manipulation of higher order transverse spatial modes for the purposes of quantum information processing. We propose two such applications: the production of both spatial-mode entangled Bell states and heralded single photons, tailored to cover the entire Poincaré sphere of first-order transverse modes. In addition to the aforementioned transverse spatial manipulation based on free-space parity sorting, we introduce several more such techniques involving photons propagating in optical fibers. We show that when a photon propagates in a cylindrically symmetric waveguide, its spin angular momentum and its orbital angular momentum (OAM) interact. This spin-orbit interaction (SOI) leads to the prediction of several novel rotational effects: the spatial or time evolution of the photonic polarization vector is controlled by its OAM quantum number or, conversely, its spatial wave function is controlled by its spin. We demonstrate how these phenomena can be used to reversibly transfer entanglement between the spin and OAM degrees of freedom of two-particle states. In order to provide a deeper insight into the cause of the SOI for photons, we also investigate an analogous interaction for electrons in a cylindrical waveguide and find that each of the SOI effects mentioned above remain manifest for the electron case. We show that the SOI dynamics are quantitatively described by a single expression applying to both electrons and photons and explain their common origin in terms of a universal geometric phase associated with the interplay between either particle's spin and OAM. This implies that these SOI-based effects occur for any particle with spin and thereby exist independently of whether or not the particle has mass, charge, or magnetic moment. / Committee in charge: Daniel Steck, Chairperson, Physics; Michael Raymer, Member, Physics; Jens Noeckel, Member, Physics; Steven van Enk, Member, Physics; Andrew Marcus, Outside Member, Chemistry

Les évolutions rapides du marché des composants électroniques font apparaître de nombreux challenges pour la conception et la fabrication de ces derniers. Lorsque ces éléments deviennent plus petits, leur comportement se complexifie à mesure que de nouveaux phénomènes, liés aux effets d'interférence, entrent en jeu. Comprendre ces derniers nécessite le développement d'outils théoriques avancés. Dans ce contexte cette thèse est consacrée au transport électronique quantique dans des systèmes multi-terminaux. Dans la première partie on développe un formalisme général, utilisant les fonctions de Green de Keldysh, pour le transport électronique quantique dans des systèmes multi-terminaux en présence de perturbations oscillantes. Nous sommes capable d'exprimer toute obervable AC en termes de fonctions de Green à l'équilibre et des self-énergies des contacts. Ceci fait de notre formalisme un outil pratique pour toute une variété de perturbations à fréquence finie. Dans la seconde partie on présente l'idée d'induction d'un fort couplage spin-orbite dans le graphène en déposant à sa surface un certain type d'atomes lourds. Le graphène devient alors un isolant topologique. Nous avons ensuite étudié l'évolution de la phase topologique avec un champ magnétique externe. Une transition entre la phase de Hall quantique et la phase de Hall quantique de spin a été identifiée dans le même système en variant seulement la position du niveau de Fermi. Nous avons montré qu'une hétérojonction entre ces deux phases donnait lieu à un nouveau type d'état chiral à l'interface. / Rapidly changing market of electronic devices sets up a lot of challenges for the manufacturing and design technologies. When electronic circuit elements get smaller, the device behavior becomes increasingly complicated as new physical phenomena due to quantum interference effects come into play. Understanding of the latter necessitates development of advanced theoretical tools. In this thesis we investigate quantum electron transport in multiterminal devices. In the first part making use of the Keldysh Green's functions we develop a general framework for electron quantum transport in multi-terminal systems in the presence of oscillating fields. We are able to express any AC observable in terms of stationary Green's functions and leads self-energies, which makes our formalism a practical numerical tool for a variety of possible finite-frequency perturbations. In the second part we investigate theoretically a proposal to induce strong spin-orbital coupling in graphene by functionalizing its surface with certain type of heavy adatoms. In this case graphene becomes a topological insulator. Then we investigate the evolution of this topological phase in external magnetic field. We were able to see a unique transition between quantum Hall and quantum spin Hall phases in the same system by only varying the position of the Fermi level. A heterojunction between these two phases was shown to give rise to a new type of a chiral state at the interface between the latter.