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Bulk-boundary correspondence is a foundational principle underlying the electronic band structure and physical behavior of topological quantum materials. Although it has been rigorously tested in topological systems where the physical properties involve charge currents, it remains unclear whether bulk-boundary correspondence should also hold for non-conserved spin currents. We study charge-to-spin conversion in a canonical topological insulator, Bi$_{1-x}$Sb$_x$, to address this fundamentally unresolved question. We use spin-torque ferromagnetic resonance measurements to accurately probe the charge-to-spin conversion efficiency in epitaxial Bi$_{1-x}$Sb$_x$~thin films of high structural quality spanning the entire range of composition, including both trivial and topological band structures, as verified using {\it in vacuo} angle-resolved photoemission spectroscopy. From these measurements, we deduce the effective spin Hall conductivity (SHC) and find excellent agreement with the values predicted by tight-binding calculations for the intrinsic SHC of the bulk bands. These results provide strong evidence that the strong spin-orbit entanglement of bulk states well below the Fermi energy connects directly to the SHC in epitaxial Bi$_{1-x}$Sb$_x$~films interfaced with a metallic ferromagnet. The excellent agreement between theory and experiment points to the generic value of analyses focused entirely on bulk properties, even for topological systems involving non-conserved spin currents.

We present a first-principles study of defect formation and electronic structure of erbium (Er)-doped yttria (Y$_2$O$_3$). This is an emerging material for spin-photon interfaces in quantum information science due to the narrow linewidth optical emission from Er dopants at standard telecommunication wavelengths and their potential for quantum memories and transducers. We calculate formation energies of neutral, negatively, and positively charged Er dopants and find the charge neutral configuration to be the most stable, consistent with experiment. Of the two substitutional sites of Er for Y, the $C_2$ (more relevant for quantum memories) and $C_{3i}$ (more relevant for quantum transduction), we identify the former as possessing the lowest formation energy. The electronic properties are calculated using the Perdew-Burke-Ernzerhof (PBE) functional along with the Hubbard $U$ parameter and spin-orbit coupling (SOC), which yields a $\sim$ 6 $\mu_B$ orbital and a $\sim$ 3 $\mu_B$ spin magnetic moment, and 11 electrons in the Er $4f$ shell, confirming the formation of charge-neutral Er$^{3+}$. This standard density functional theory (DFT) approach underestimates the band gap of the host and lacks a first-principles justification for $U$. To overcome these issues, we performed screened hybrid functional (HSE) calculations, including a negative $U$ for the $4f$ orbitals, with mixing ($\alpha$) and screening ($w$) parameters. These produced robust electronic features with slight modifications in the band gap and the $4f$ splittings depending on the choice of tuning parameters. We also computed the many-particle electronic excitation energies and compared them with experimental values from photoluminescence., Comment: 9 pages, 6 figures

Copper-doped zinc sulfide (ZnS:Cu) exhibits down-conversion luminescence in the UV, visible, and IR regions of the electromagnetic spectrum; the visible red, green, and blue emission is referred to as R-Cu, G-Cu, and B-Cu, respectively. The sub-bandgap emission arises from optical transitions between localized electronic states created by point defects, making ZnS:Cu a prolific phosphor material and an intriguing candidate material for quantum information science, where point defects excel as single-photon sources and spin qubits. Colloidal nanocrystals (NCs) of ZnS:Cu are particularly interesting as hosts for the creation, isolation, and measurement of quantum defects, since their size, composition, and surface chemistry can be precisely tailored for bio-sensing and opto-electronic applications. Here, we present a method for synthesizing colloidal ZnS:Cu NCs that emit primarily R-Cu, which has been proposed to arise from the Cu$_{Zn}$-V$_S$ complex, an impurity-vacancy point defect structure analogous to well-known quantum defects in other materials that produce favorable optical and spin dynamics. First principles calculations confirm the thermodynamic stability and electronic structure of Cu$_{Zn}$-V$_S$. Temperature- and time-dependent optical properties of ZnS:Cu NCs show blueshifting luminescence and an anomalous plateau in the intensity dependence as temperature is increased from 19 K to 290 K, for which we propose an empirical dynamical model based on thermally-activated coupling between two manifolds of states inside the ZnS bandgap. Understanding of R-Cu emission dynamics, combined with a controlled synthesis method for obtaining R-Cu centers in colloidal NC hosts, will greatly facilitate the development of Cu$_{Zn}$-V$_S$ and related complexes as quantum point defects in ZnS., Comment: 31 pages, 19 figures

Thermoelectric modules are a promising approach to energy harvesting and efficient cooling. In addition to the longitudinal Seebeck effect, recently transverse devices utilizing the anomalous Nernst effect (ANE) have attracted interest. For high conversion efficiency, it is required that the material should have a large ANE thermoelectric power and low electrical resistance, the product of which is the ANE conductivity. ANE is usually explained in terms of intrinsic contributions from Berry curvature. Our observations suggest that extrinsic contributions also matter. Studying single-crystal MnBi, we find a very high ANE thermopower (~10 $\mu$V/K) under 0.6 T at 80 K, and a transverse thermoelectric conductivity of over 40 A/Km. With insight from theoretical calculations, we attribute this large ANE predominantly to a new advective magnon contribution arising from magnon-electron spin-angular momentum transfer. We propose that introducing large spin-orbit coupling into ferromagnetic materials may enhance the ANE through the extrinsic contribution of magnons., Comment: 14 pages, 4 figures

One of the most fundamental and exotic properties of 3D topological insulators (TIs) is spin-momentum-locking (SML) of their topological surface states (TSSs), promising for potential applications in future spintronics. However, other possible conduction channels, such as a trivial two-dimensional electron gas (2DEG) with strong Rashba type spin-orbit interaction (SOI) and bulk conducting states that may possess a spin Hall effect (SHE), can coexist in 3D TIs, making determining the origin of the current induced spin polarization (CISP) difficult. In this work, we directly compared the CISP between bulk-insulating Bi2Te2Se (BTS221) and bulk-metallic Bi2Se3 thin flakes using spin potentiometry. In the bulk insulating BTS221, the observed CISP has a sign consistent with the expected helicity of the SML of the TSS, but an opposite sign to its calculated bulk spin Hall conductivity (SHC). However, compared to BTS221, an opposite CISP is observed in the bulk metallic Bi2Se3, consistent instead with both the expectations of its Rashba-Edelstein effect of the band-bending induced 2DEG and bulk spin Hall Effect (SHE). Our results provide an electrical way to distinguish the TSS from other possible conducting channels in spin transport measurements on 3D TIs, and open ways for the potential applications in charge-spin conversion devices., Comment: 15 pages, 6 figures

The chiral anomaly is the predicted break down of chiral symmetry in a Weyl semimetal with monopoles of opposite chirality when an electric field parallel to a magnetic field is applied. It occurs because of charge pumping from a positive chirality to a negative chirality monopole. Experimental observation of this fundamental effect has been plagued by concerns about the pathways of the current. Here, we unambiguously demonstrate the thermal analog of the chiral anomaly in topological insulator bismuth-antimony alloys driven into an ideal Weyl semimetal state by a Zeeman field, with the chemical potential pinned at the Weyl points, and in which the Fermi surface has no trivial pockets. The experimental signature is a large enhancement of the thermal conductivity in an applied magnetic field parallel to the thermal gradient that follows the Wiedemann-Franz law above 60 K. Absence of current flow avoids extrinsic effects that plague electrical measurements., Comment: 25 pages, 4 figures

The intrinsic spin Hall conductivity of a two-dimensional gas confined to SrTiO$_3$, such as occurs at an LaAlO$_3$/SrTiO$_3$ interface, is calculated from the Kubo formula. The effect of strain in the [001] (normal to the quantum well direction) and the [111] direction is incorporated into a full tight-binding Hamiltonian. We show that the spin-charge conversion ratio can be significantly altered through strain and gate voltage by tuning the chemical potential. Strain direction is also a significant factor in the spin Hall response as this direction affects the alignment of the conduction bands., Comment: 9 pages, 6 figures

This thesis predicts that two types of material families could be a solution to the challenges in spintronics: complex oxides and bismuth based materials. We derive a general approach for constructing an effective spin-orbit Hamiltonian, which applies to all nonmagnetic materials. We also verify this formalism through comparisons with other approaches for III-V semiconductors. Its general applicability is illustrated by deriving the spin-orbit interaction and predicting spin lifetimes for strained SrTiO$_3$ and a two-dimensional electron gas (such as at the LaAlO$_3$/SrTiO$_3$ interface). Our results suggest robust spin coherence and spin transport properties in SrTiO$_3$ related materials. In the second part, we calculate intrinsic spin Hall conductivities for Bi$_{1-x}$Sb$_x$ semimetals with strong spin-orbit couplings, from the Kubo formula and using Berry curvatures evaluated from a tight-binding Hamiltonian. Nearly crossing bands with strong spin-orbit interaction generate giant spin Hall conductivities in these materials, ranging from 474 ($\hbar/e)( \Omega^{-1}cm^{-1}$) for bismuth to 96($\hbar/e)( \Omega^{-1}cm^{-1}$) for antimony; the value for bismuth is more than twice that of platinum. The large spin Hall conductivities persist for alloy compositions corresponding to a three-dimensional topological insulator state, such as Bi$_{0.83}$Sb$_{0.17}$. The spin Hall conductivity could be changed by a factor of 5 for doped Bi, or for Bi$_{0.83}$Sb$_{0.17}$, by changing the chemical potential, suggesting the potential for doping or voltage tuned spin Hall current. We also calculate intrinsic spin Hall conductivities of Bi$_2$Se$_3$ and Bi$_2$Te$_3$ topological insulators from an effective tight-binding Hamiltonian. We conclude that bismuth-antimony alloys and bismuth chalcogenides are primary candidates for efficiently generating spin currents through the spin Hall effect., Comment: Thesis defended in July 15, 2015 at the University of Iowa

Intrinsic spin Hall conductivities are calculated for strong spin-orbit Bi$_{1-x}$Sb$_x$ semimetals, from the Kubo formula and using Berry curvatures evaluated throughout the Brillouin zone from a tight-binding Hamiltonian. Nearly-crossing bands with strong spin-orbit interaction generate giant spin Hall conductivities in these materials, ranging from 474 ($\hbar$/e)($\Omega$cm)$^{-1}$ for bismuth to 96 ($\hbar$/e)($\Omega$cm)$^{-1}$ for antimony; the value for bismuth is more than twice that of platinum. The large spin Hall conductivities persist for alloy compositions corresponding to a three-dimensional topological insulator state, such as Bi$_{0.83}$Sb$_{0.17}$. The spin Hall conductivity could be changed by a factor of five for doped Bi, or for Bi$_{0.83}$Sb$_{0.17}$, by changing the chemical potential by 0.5 eV, suggesting the potential for doping or voltage tuned spin Hall current.

A general approach is derived for constructing an effective spin-orbit Hamiltonian for nonmagnetic materials, which is useful for calculating spin-dependent properties near an arbitrary point in momentum space with pseudospin degeneracy. The formalism is verified through comparisons with other approaches for III-V semiconductors, and its general applicability is illustrated by deriving the spin-orbit interaction and predicting spin lifetimes for strained SrTiO$_3$ and a two-dimensional electron gas in SrTiO$_3$ (such as at the LaAlO$_3$/SrTiO$_3$ interface). These results suggest robust spin coherence and spin transport properties in SrTiO$_3$-based materials at room temperature., Comment: Published 2 April 2014