Engineering Quantum Spin Hall Effect in Graphene Nanoribbons via Edge Functionalization

Kane and Mele predicted that in presence of spin-orbit interaction graphene realizes the quantum spin Hall state. However, exceptionally weak intrinsic spin-orbit splitting in graphene ($\approx 10^{-5}$ eV) inhibits experimental observation of this topological insulating phase. To circumvent this problem, we propose a novel approach towards controlling spin-orbit interactions in graphene by means of covalent functionalization of graphene edges with functional groups containing heavy elements. Proof-of-concept first-principles calculations show that very strong spin-orbit coupling can be induced in realistic models of narrow graphene nanoribbons with tellurium-terminated edges. We demonstrate that electronic bands with strong Rashba splitting as well as the quantum spin Hall state spanning broad energy ranges can be realized in such systems. Our work thus opens up new horizons towards engineering topological electronic phases in nanostructures based on graphene and other materials by means of locally introduced spin-orbit interactions.Comment: 5 pages, 3 figure

Electronic properties of one-dimensional nanostructures of the Bi2_2Se3_3 topological insulator

We theoretically study the electronic structure and spin properties of one-dimensional nanostructures of the prototypical bulk topological insulator Bi$_2$Se$_3$. Realistic models of experimentally observed Bi$_2$Se$_3$ nanowires and nanoribbons are considered using the tight-binding method. At low energies, the band structures are composed of a series of evenly spaced degenerate sub-bands resulting from circumferential confinement of the topological surface states. The direct band gaps due to the non-trivial $\pi$ Berry phase show a clear dependence on the circumference. The spin-momentum locking of the topological surface states results in a pronounced 2$\pi$ spin rotation around the circumference with the degree of spin polarization dependent on the the momentum along the nanostructure. Overall, the band structures and spin textures are more complicated for nanoribbons, which expose two distinct facets. The effects of reduced dimensionality are rationalized with the help of a simple model that considers circumferential quantization of the topological surface states. Furthermore, the surface spin density induced by electric current along the nanostructure shows a pronounced oscillatory dependence on the charge-carrier energy, which can be exploited in spintronics applications.Comment: 10 pages, 9 figure

Orbital contribution to the magnetic properties of iron as a function of dimensionality

The orbital contribution to the magnetic properties of Fe in systems of decreasing dimensionality (bulk, surfaces, wire and free clusters) is investigated using a tight-binding hamiltonian in an $s, p,$ and $d$ atomic orbital basis set including spin-orbit coupling and intra-atomic electronic interactions in the full Hartree-Fock (HF) scheme, i.e., involving all the matrix elements of the Coulomb interaction with their exact orbital dependence. Spin and orbital magnetic moments and the magnetocrystalline anisotropy energy (MAE) are calculated for several orientations of the magnetization. The results are systematically compared with those of simplified hamiltonians which give results close to those obtained from the local spin density approximation. The full HF decoupling leads to much larger orbital moments and MAE which can reach values as large as 1$\mu_B$ and several tens of meV, respectively, in the monatomic wire at the equilibrium distance. The reliability of the results obtained by adding the so-called Orbital Polarization Ansatz (OPA) to the simplified hamiltonians is also discussed. It is found that when the spin magnetization is saturated the OPA results for the orbital moment are in qualitative agreement with those of the full HF model. However there are large discrepancies for the MAE, especially in clusters. Thus the full HF scheme must be used to investigate the orbital magnetism and MAE of low dimensional systems

Multiplet features and magnetic properties of Fe on Cu(111): From single atoms to small clusters

The observation of sharp atomiclike multiplet features is unexpected for individual 3d atoms adsorbed on transition-metal surfaces. However, we show by means of x-ray absorption spectroscopy and x-ray magnetic circular dichroism that individual Fe atoms on Cu(111) exhibit such features. They are reminiscent of a low degree of hybridization, similar to 3d atoms adsorbed on alkali-metal surfaces. We determine the spin, orbital, and total magnetic moments, as well as magnetic anisotropy energy for the individual Fe atoms and for small Fe clusters that we form by increasing the coverage. The multiplet features are smoothened and the orbital moment rapidly decreases with increasing cluster size. For Fe monomers, comparison with density functional theory and multiplet calculations reveals a d(7) electronic configuration, owing to the transfer of one electron from the 4s to the 3d states

Localized electronic states at grain boundaries on the surface of graphene and graphite

Recent advances in large-scale synthesis of graphene and other 2D materials have underscored the importance of local defects such as dislocations and grain boundaries (GBs), and especially their tendency to alter the electronic properties of the material. Understanding how the polycrystalline morphology affects the electronic properties is crucial for the development of applications such as flexible electronics, energy harvesting devices or sensors. We here report on atomic scale characterization of several GBs and on the structural-dependence of the localized electronic states in their vicinity. Using low temperature scanning tunneling microscopy (STM) and spectroscopy (STS), together with tight binding and ab initio numerical simulations we explore GBs on the surface of graphite and elucidate the interconnection between the local density of states (LDOS) and their atomic structure. We show that the electronic fingerprints of these GBs consist of pronounced resonances which, depending on the relative orientation of the adjacent crystallites, appear either on the electron side of the spectrum or as an electron-hole symmetric doublet close to the charge neutrality point. These two types of spectral features will impact very differently the transport properties allowing, in the asymmetric case to introduce transport anisotropy which could be utilized to design novel growth and fabrication strategies to control device performance

A Novel Quasi-One-Dimensional Topological Insulator in Bismuth Iodide β\beta-Bi4_4I4_4

Recent progress in the field of topological states of matter(1,2) has largely been initiated by the discovery of bismuth and antimony chalcogenide bulk topological insulators (TIs)(3-6), followed by closely related ternary compounds(7-16) and predictions of several weak TIs(17-19). However, both the conceptual richness of Z$_2$ classification of TIs as well as their structural and compositional diversity are far from being fully exploited. Here, a new Z$_2$ topological insulator is theoretically predicted and experimentally confirmed in the $\beta$-phase of quasi-one-dimensional bismuth iodide Bi$_4$I$_4$. The electronic structure of $\beta$-Bi$_4$I$_4$, characterized by Z$_2$ invariants (1;110), is in proximity of both the weak TI phase (0;001) and the trivial insulator phase (0;000). Our angle-resolved photoemission spectroscopy measurements on the (001) surface reveal a highly anisotropic band-crossing feature located at the point of the surface Brillouin zone and showing no dispersion with the photon energy, thus being fully consistent with the theoretical prediction

Transport électronique polarisé en spin dans les contacts atomiques de fer

This thesis is dedicated to the theoretical study of spin-dependent transport in atomic contact. The main objective is to understand the giant anisotropic magnetoresistance experimentally measured in iron break junctions. On this purpose, we developed a method to calculate electron transport properties in magnetic nanostructures. The calculation is performed in two steps. First the electronic structure of the contact is determined in a basis of atomic orbitals spd using a tight-binding model extended to include magnetism. The magnetic properties are described at the atomic scale using an interelectronic interaction Hamiltonian. Two interaction models are compared : a simple Stoner-like model and a more complete Hartree-Fock model, developed to reproduce the orbital polarization effects which appear in one-dimensional nanostructure. To describe the magnetic anisotropy, noncollinear magnetism and spin-orbit coupling are taken in account. In the second step, the electron transport properties are derived in the Landauer formalism. In this approach, the transport of electron is supposed to be coherent and elastic. The conductance is directly proportional to the transmission probability of electrons through the contact. This transmission is calculated from the Green function of the system. This method is applied to the study of magnetoresistance in iron atomic contact. Several contact geometries, from the monatomic wire to realistic systems, are compared. The results reveal the importance of contact geometry and orbital polarization.Cette thèse est consacrée à l'étude théorique du transport électronique dans les contacts atomiques magnétiques. L'objectif principal est d'expliquer la magnétorésistance anisotrope géante mesurée expérimentalement dans les jonctions à cassure de fer. Dans ce but, on a développé une méthode de calcul de la conductance des nanostructures magnétiques.Le calcul est effectué en deux étapes. Dans un premier temps, la structure électronique du contact est déterminée de manière autocohérente dans une base d'orbitales atomiques spd à l'aide d'un modèle de liaisons fortes étendu au magnétisme. Les propriétés magnétiques sont décrites à l'échelle atomique par un modèle d'interaction inter-électronique. Deux modèles d'interactions sont comparés : un modèle simple de type Stoner et un modèle plus complet de type Hartree-Fock développé pour reproduire les effets de polarisation orbitale susceptibles d'apparaître au niveau du contact. En effet, dans les nanostructures unidimensionnelles, on observe une levée du blocage du moment orbital qui existe dans les cristaux cubiques en volume. Pour permettre la description de l'anisotropie magnétique du système, on prend aussi en compte le magnétisme non-colinéaire et le couplage spin-orbite.Dans un second temps, les propriétés de transport électroniques du système sont déterminées dans le formalisme de Landauer. Dans cette approche, on considère que le transport est cohérent et élastique. Cette approximation est valide quand étudie un conducteur de taille atomique à basse température sous de faibles tensions. La conductance est alors directement proportionnelle à la probabilité de transmission des électrons à travers le système. Cette transmission est calculée à partir de la fonction de Green du système. Cette méthode de calcul est appliquée à l'étude de la magnétorésistance anisotrope des contacts de fer. Plusieurs géométries de contact, allant du fil monoatomique parfait aux systèmes réalistes, sont comparées. Les résultats révèlent le rôle prépondérant joué par la géométrie et par la polarisation orbitale. Pour que l'anisotropie magnétique soit aussi élevée que dans les expériences, il est nécessaire que l'atome de contact soit dans une configuration de fil monoatomique. Les effets de polarisation orbitale permettent d'expliquer les deux plateaux de conductance mesurés expérimentalement. Ils sont liés à l'existence de deux états magnétiques métastables qui différent par la direction du moment orbital sur l'atome de contact