arXiv subjects

Steven G. Louie

Publications and source records attributed to Steven G. Louie.

At least 109 records · Page 6Linked to original sources

arXiv2017

Alternative structure of TiO2 with higher energy valence band edge

We propose an alternative structure of TiO2 anatase that has a higher energy oxygen p-like valence band maximum than the pristine TiO2 anatase and thus has a much better alignment with the water splitting levels. This alternative structure is unique when considering a large subspace of possible structural distortions of TiO2 anatase. We propose two routes towards this state and argue that one of them might have been realized in the recently discovered so-called black TiO2.

cond-mat.mtrl-sci↗

arXiv2017

Topological Phases in Graphene Nanoribbons: Junction States, Spin Centers and Quantum Spin Chains

Knowledge of the topology of the electronic ground state of materials has led to deep insights to novel phenomena such as the integer quantum Hall effect and fermion-number fractionalization, as well as other properties of matter. Joining two insulators of different topological classes produces fascinating boundary states in the band gap. Another exciting recent development is the bottom-up synthesis (from molecular precursors) of graphene nanoribbons (GNRs) with atomic precision control of their edge and width. Here we connect these two fields, and show for the first time that semiconducting GNRs of different width, edge, and end termination belong to different topological classes. The topology of GNRs is protected by spatial symmetries and dictated by the terminating unit cell. We have derived explicit formula for their topological invariants, and show that localized junction states developed between two GNRs of distinct topology may be tuned by lateral junction geometry. The topology of a GNR can be further modified by dopants, such as a periodic array of boron atoms. In a superlattice consisted of segments of doped and pristine GNRs, the junction states are stable spin centers, forming a Heisenberg antiferromagnetic spin 1/2 chain with tunable exchange interaction. The discoveries here are not only of scientific interest for studies of quasi one-dimensional systems, but also open a new path for design principles of future GNR-based devices through their topological characters.

cond-mat.mes-hall↗

arXiv2017

Gate Switchable Transport and Optical Anisotropy in 90° Twisted Bilayer Black Phosphorus

Anisotropy describes the directional dependence of a material's properties such as transport and optical response. In conventional bulk materials, anisotropy is intrinsically related to the crystal structure, and thus not tunable by the gating techniques used in modern electronics. Here we show that, in bilayer black phosphorus with an interlayer twist angle of 90°, the anisotropy of its electronic structure and optical transitions is tunable by gating. Using first-principles calculations, we predict that a laboratory-accessible gate voltage can induce a hole effective mass that is 30 times larger along one Cartesian axis than along the other axis, and the two axes can be exchanged by flipping the sign of the gate voltage. This gate-controllable band structure also leads to a switchable optical linear dichroism, where the polarization of the lowest-energy optical transitions (absorption or luminescence) is tunable by gating. Thus, anisotropy is a tunable degree of freedom in twisted bilayer black phosphorus.

cond-mat.mtrl-sci↗

arXiv2017

Insulating titanium oxynitride for visible light photocatalysis

We propose a systematic approach to obtain various forms of insulating titanium oxynitrides Ti$_{n}$N$_{2}$O$_{2n-3}$ and we conduct a detailed study on its $n=2$ case, Ti$_{2}$N$_{2}$O. We study the energetics and the electronic structures of Ti$_{2}$N$_{2}$O and compare these results with those of pristine and nitrogen-doped TiO$_{2}$ within the framework of the density-functional theory (DFT) and the GW approximation. We find that Ti$_{2}$N$_{2}$O is semiconducting with the calculated band-gap of 1.81 eV, which is significantly smaller than those of pristine TiO$_{2}$ rutile (3.14 eV) or anatase (3.55 eV). Furthermore, the reduction of the band-gap of Ti$_{2}$N$_{2}$O is realized not by lowering of the conduction-band minimum but by rising the valence-band maximum. Therefore the proposed Ti$_{2}$N$_{2}$O has suitable band-edge alignment for water-splitting photocatalysis. Finally, total energy calculations indicate that Ti$_{2}$N$_{2}$O is potentially easier to synthesize than nitrogen-doped TiO$_{2}$. Based on these results, we propose Ti$_{2}$N$_{2}$O as a promising visible-light photocatalytic material.

cond-mat.mtrl-sci↗

arXiv2016

Magnetic brightening and control of dark excitons in monolayer WSe2

Monolayer transition metal dichalcogenide (TMDC) crystals, as direct-gap materials with unusually strong light-matter interaction, have attracted much recent attention. In contrast to the initial understanding, the minima of the conduction band are predicted to be spin split. Because of this splitting and the spin-polarized character of the valence bands, the lowest-lying excitonic states in WX2 (X=S, Se) are expected to be spin-forbidden and optically dark. To date, however, there has been no direct experimental probe of these dark band-edge excitons, which strongly influence the light emission properties of the material. Here we show how an in-plane magnetic field can brighten the dark excitonic states and allow their properties to be revealed experimentally in monolayer WSe2. In particular, precise energy levels for both the neutral and charged dark excitons were obtained and compared with ab-initio calculations using the GW-BSE approach. Greatly increased emission and valley lifetimes were observed for the brightened dark states as a result of their spin configuration. These studies directly probe the excitonic spin manifold and provide a new route to tune the optical and valley properties of these prototypical two-dimensional semiconductors.

cond-mat.mes-hall↗

arXiv2016

Anomalous localization behaviors in disordered pseudospin systems: Beyond the conventional Anderson picture

We discovered novel Anderson localization behaviors of pseudospin systems in a 1D disordered potential. For a pseudospin-1 system, due to the absence of backscattering under normal incidence and the presence of a conical band structure, the wave localization behaviors are entirely different from those of normal disordered systems. We show both numerically and analytically that there exists a critical strength of random potential ($W_c$), which is equal to the incident energy ($E$), below which the localization length $ξ$ decreases with the random strength $W$ for a fixed incident angle $θ$. But the localization length drops abruptly to a minimum at $W=W_c$ and rises immediately afterwards, which has never been observed in ordinary materials. The incidence angle dependence of the localization length has different asymptotic behaviors in two regions of random strength, with $ξ\propto \sin^{-4}θ$ when $W W_c$. Experimentally, for a given disordered sample with a fixed randomness strength $W$, the incident wave with incident energy $E$ will experience two different types of localization, depending on whether $E>W$ or $E<W$. The existence of a sharp transition at $E=W$ is due to the emergence of evanescent waves in the systems when $E<W$. Such localization behavior is unique to pseudospin-1 systems. For pseudospin-1/2 systems, there is a minimum localization length as randomness increases, but the transition from decreasing to increasing localization length at the minimum is smooth rather than abrupt. In both decreasing and increasing regions, the $θ$ -dependence of the localization length has the same asymptotic behavior $ξ\propto \sin^{-2}θ$.

cond-mat.dis-nn↗

arXiv2016

Effective Mass in Bilayer Graphene at Low Carrier Densities: the Role of Potential Disorder and Electron-Electron Interaction

In a two-dimensional electron gas, the electron-electron interaction generally becomes stronger at lower carrier densities and renormalizes the Fermi liquid parameters such as the effective mass of carriers. We combine experiment and theory to study the effective masses of electrons and holes $m^*_e$ and $m^*_h$ in bilayer graphene in the low carrier density regime of order 1 * 10^11 cm^-2. Measurements use temperature-dependent low-field Shubnikov-de Haas (SdH) oscillations are observed in high-mobility hexagonal boron nitride (h-BN) supported samples. We find that while $m^*_e$ follows a tight-binding description in the whole density range, $m^*_h$ starts to drop rapidly below the tight-binding description at carrier density n = 6 * 10^11 cm^-2 and exhibits a strong suppression of 30% when n reaches 2 * 10^11 cm^-2. Contributions from electron-electron interaction alone, evaluated using several different approximations, cannot explain the experimental trend. Instead, the effect of potential fluctuation and the resulting electron-hole puddles play a crucial role. Calculations including both the electron-electron interaction and disorder effects explain the experimental data qualitatively and quantitatively. This study reveals an unusual disorder effect unique to two-dimensional semi-metallic systems.

cond-mat.mes-hall↗

arXiv2016

Non-uniform sampling schemes of the Brillouin zone for many-electron perturbation-theory calculations in reduced dimensionality

First principles calculations based on many-electron perturbation theory methods, such as the \textit{ab initio} GW and GW plus Bethe-Salpeter equation (GW-BSE) approach, are reliable ways to predict quasiparticle and optical properties of materials, respectively. However, these methods involve more care in treating the electron-electron interaction and are considerably more computationally demanding when applied to systems with reduced dimensionality, since the electronic confinement leads a slower convergence of sums over the Brillouin zone due to a much more complicated screening environment that manifests in the "head" and "neck" elements of the dielectric matrix. Here, we present two new schemes to sample the Brillouin zone for GW and GW-BSE calculations: the non-uniform neck subsampling method and the clustered sampling interpolation method, which can respectively be used for a family of single-particle problems, such as GW calculations, and for problems involving the scattering of two-particle states, such as when solving the BSE. We tested these methods on several few-layer semiconductors and graphene and show that they perform a much more efficient sampling of the Brillouin zone and yield two to three orders of magnitude reduction in the computer time. These two methods can be readily incorporated into several \textit{ab initio} packages that compute electronic and optical properties through the GW and GW-BSE approaches.

cond-mat.mtrl-sci↗

arXiv2016

Generation of Anisotropic Massless Dirac Fermions and Asymmetric Klein Tunneling in Few-Layer Black Phosphorus Superlattices

Artificial lattices have been employed in many two-dimensional systems, including those of electrons, atoms and photons, in a quest for massless Dirac particles with flexibility and controllability. Periodically patterned molecule assembly and electrostatic gating as well as moiré pattern induced by substrate, have produced electronic states with linear dispersions from isotropic two-dimensional electron gas (2DEG). Here we demonstrate that massless Dirac fermions with tunable anisotropic characteristics can, in general, be generated in highly anisotropic 2DEG under slowly varying external periodic potentials. For patterned few-layer black phosphorus superlattices, the new chiral quasiparticles exist exclusively in an isolated energy window and inherit the strong anisotropic properties of pristine black phosphorus. These states exhibit asymmetric Klein tunneling with the direction of incidence for wave packet with perfect transmission deviating from normal incidence by more than 50° under an appropriate barrier orientation.

cond-mat.mtrl-sci↗

arXiv2016

Antiferromagnetism enables electron-phonon coupling in iron-based superconductors

It is shown that a generic form of an antiferromagnetic wave function opens strong electron-phonon coupling channels in the iron-based superconductors. In the nonmagnetic state these channels exist locally on a single iron atom, but are canceled out between the two iron atoms in the primitive unit cell. Our findings are based on symmetry and the presence of an xz/yz Fermi surface near the M point and thus should be relevant for the known iron-based pnictide or chalcogenide superconductors.

cond-mat.supr-con↗

arXiv2016

Temperature-induced topological phase transitions: promoted vs. suppressed non-trivial topology

We determine the topological phase diagram of BiTl(S$_{1-δ}$Se$_δ$)$_2$ as a function of doping and temperature from first-principles calculations. Due to electron\textendash phonon interaction, the bands are renormalized at finite temperature, allowing for a transition between the trivial ($Z_2=0$) and non-trivial ($Z_2=1$) topological phase. We find two distinct regions of the phase diagram with non-trivial topology. In BiTlS$_2$, the phonons promote the crystal to the topological phase at high temperature, while in BiTlSe$_2$, the topological phase exists only at low temperature. This behaviour is explained by the symmetry of the phonon coupling potential, whereby the even phonon modes (whose potential is even under inversion) promote the topological phase and the odd phonon modes promote the trivial phase.

cond-mat.mes-hall↗

arXiv2016

Automated construction of maximally localized Wannier functions for bands with nontrivial topology

We show that an optimized projection functions method can automatically construct maximally localized Wannier functions even for bands with nontrivial topology. We demonstrate this method on a tight-binding model of a two-dimensional $\mathbb{Z}_2$ topological insulator, on a three-dimensional strong $\mathbb{Z}_2$ topological insulator, as well as on first-principles density functional theory calculated valence states of Bi$_2$Se$_3$. In all cases, the resulting Wannier functions contain large imaginary components and are more extended than those in the topologically trivial phase.

cond-mat.mtrl-sci↗

arXiv2016

Proposal for a bulk material based on a monolayer FeSe on SrTiO3 high-temperature superconductor

Motivated by the high superconducting transition temperature of monolayer FeSe on SrTiO3, we propose a potential three-dimensional high-temperature superconductor superlattice FeSe-SrTiO3 and study its structural stability and electronic structure using density functional theory. We find that the binding energy between the FeSe and SrTiO3 layers is about 0.7 eV per (Fe2Se2) unit and that it saturates already within a single TiO2 atomic layer of SrTiO3. In addition we analyzed the dynamical stability of the superlattice and compared it to the case of bulk SrTiO3.

cond-mat.supr-con↗

arXiv2016

Dispersion and lineshape of plasmon satellites in one, two and three dimensions

Using state-of-the-art many-body Green's function calculations based on the "GW plus cumulant" approach, we analyze the properties of plasmon satellites in the electron spectral function resulting from electron-plasmon interactions in one-, two- and three-dimensional systems. Specifically, we show how their dispersion relation, lineshape and linewidth are related to the properties of the constituent electrons and plasmons. To gain insight into the many-body processes giving rise to the formation of plasmon satellites, we connect the "GW plus cumulant" approach to a many-body wavefunction picture of electron-plasmon interactions and introduce the coupling-strength weighted electron-plasmon joint-density states as a powerful concept for understanding plasmon satellites.

cond-mat.mes-hall↗

arXiv2016

Screening and Many-Body Effects in Two-Dimensional Crystals: Monolayer MoS$_{2}$

We present a systematic study of the variables affecting the electronic and optical properties of two-dimensional(2D) crystals within \textit{ab initio} GW and GW plus Bethe Salpeter Equation (GW-BSE) calculations. As a prototypical 2D transition metal dichalcogenide material, we focus our study on monolayer MoS${}_2$. We find that the reported variations in GW-BSE results in the literature for monolayer MoS${}_2$ and related systems arise from different treatments of the long-range Coulomb interaction in supercell calculations and convergence of k-grid sampling and cutoffs for various quantities such as the dielectric screening. In particular, the quasi-2D nature of the system gives rise to fast spatial variations in the screening environment, which are computationally challenging to resolve. We also show that common numerical treatments to remove the divergence in the Coulomb interaction can shift the exciton continuum leading to false convergence with respect to k-point sampling. Our findings apply to GW-BSE calculations on any low-dimensional semiconductors.

cond-mat.mtrl-sci↗

arXiv2016

Low Rank Approximation in $G_0W_0$ Approximation

The single particle energies obtained in a Kohn--Sham density functional theory (DFT) calculation are generally known to be poor approximations to electron excitation energies that are measured in transport, tunneling and spectroscopic experiments such as photo-emission spectroscopy. The correction to these energies can be obtained from the poles of a single particle Green's function derived from a many-body perturbation theory. From a computational perspective, the accuracy and efficiency of such an approach depends on how a self energy term that properly accounts for dynamic screening of electrons is approximated. The $G_0W_0$ approximation is a widely used technique in which the self energy is expressed as the convolution of a non-interacting Green's function ($G_0$) and a screened Coulomb interaction ($W_0$) in the frequency domain. The computational cost associated with such a convolution is high due to the high complexity of evaluating $W_0$ at multiple frequencies. In this paper, we discuss how the cost of $G_0W_0$ calculation can be reduced by constructing a low rank approximation to the frequency dependent part of $W_0$. In particular, we examine the effect of such a low rank approximation on the accuracy of the $G_0W_0$ approximation. We also discuss how the numerical convolution of $G_0$ and $W_0$ can be evaluated efficiently and accurately by using a contour deformation technique with an appropriate choice of the contour.

math.NA↗

arXiv2016

Accurate determination of the valence band edge in hard x-ray photoemission spectra using GW theory

We introduce a new method for determining accurate values of the valence-band maximum in x-ray photoemission spectra. Specifically, we align the sharpest peak in the valence-band region of the experimental spectrum with the corresponding feature of a theoretical valence-band density of states curve from ab initio GW theory calculations. This method is particularly useful for soft and hard x-ray photoemission studies of materials with a mixture of valence-band characters, where strong matrix element effects can render standard methods for extracting the valence-band maximum unreliable. We apply our method to hydrogen-terminated boron-doped diamond, which is a promising substrate material for novel solar cell devices. By carrying out photoemission experiments with variable light polarizations, we verify the accuracy of our analysis and the general validity of the method.

cond-mat.mtrl-sci↗

arXiv2016

Klein tunneling and supercollimation of pseudospin-1 electromagnetic waves

Pseudospin plays a central role in many novel physical properties of graphene and other artificial systems which have pseudospins of 1/2. Here we show that in certain photonic crystals (PCs) exhibiting conical dispersions at k = 0, the eigenmodes near the "Dirac-like point" can be described by an effective spin-orbit Hamiltonian with a pseudospin of 1, treating wave propagations in the upper cone, the lower cone and a flat band (corresponding to zero refractive index) within a unified framework. The 3-component spinor gives rise to boundary conditions distinct from those of pseudospin-1/2, leading to new wave transport behaviors as manifested in Klein tunneling and supercollimation. For example, collimation can be realized more easily with pseudospin-1 than pseudospin-1/2. The special wave scattering properties of pseudospin-1 photons, coupled with the discovery that the effective photonic "potential" can be varied by a simple change of length scale, may offer new ways to control photon transport.

physics.optics↗