arXiv subjects

Tomáš Rauch

Publications and source records attributed to Tomáš Rauch.

16 recordsLinked to original sources

arXiv2023

Structure prediction and characterization of CuI-based ternary $p$-type transparent conductors

Zincblende copper iodide has attracted significant interest as a potential material for transparent electronics, thanks to its exceptional light transmission capabilities in the visible range and remarkable hole conductivity. However, remaining challenges hinder the utilization of copper iodide's unique properties in real-world applications. To address this, chalcogen doping has emerged as a viable approach to enhance the hole concentration in copper iodide. In search of further strategies to improve and tune the electronic properties of this transparent semiconductor, we investigate the ternary phase diagram of copper and iodine with sulphur or selenium by performing structure prediction calculations using the minima hopping method. As a result, we find 11 structures located on or near the convex hull, 9 of which are unreported. Based on our band structure calculations, it appears that sulphur and selenium are promising candidates for achieving ternary semiconductors suitable as $p$-type transparent conducting materials. Additionally, our study reveals the presence of unreported phases that exhibit intriguing topological properties. These findings broaden the scope of potential applications for these ternary systems, highlighting the possibility of harnessing their unique electronic characteristics in diverse electronic devices and systems.

cond-mat.mtrl-sci↗

arXiv2022

Favorable band alignment for photocatalysis at the strontium germanate interface with silicon

Photocatalytic water splitting is a promising strategy for large-scale clean energy production. However, efficient and low-cost solid-state photocatalysts are still lacking. We present here first-principles calculations to investigate the suitability as photocathode of an epitaxial layer of strontium germanate on a Si(100) single crystal. Conduction and valence bands offsets at the interface between these two semiconductors were determined using state-of-the-art approximations of density functional theory for the accurate prediction of band alignments. The resulting type-III band line-up is also confirmed by inspection of the spatially resolved density of states. It is concluded that the electronic structure of the investigated heterostructure is favorable for photocathodic functionality.

cond-mat.mtrl-sci↗

arXiv2022

Efficient and improved prediction of the band offsets at semiconductor heterojunctions from meta-GGA density functionals

Accurate theoretical prediction of the band offsets at interfaces of semiconductor heterostructures can often be quite challenging. Although density functional theory has been reasonably successful to carry out such calculations and efficient and accurate semilocal functionals are desirable to reduce the computational cost. In general, the semilocal functionals based on the generalized gradient approximation (GGA) significantly underestimate the bulk band gaps. This, in turn, results in inaccurate estimates of the band offsets at the heterointerfaces. In this paper, we investigate the performance of several advanced meta-GGA functionals in the computational prediction of band offsets at semiconductor heterojunctions. In particular, we investigate the performance of r2SCAN (revised strongly-constrained and appropriately-normed functional), rMGGAC (revised semilocal functional based on cuspless hydrogen model and Pauli kinetic energy density functional), mTASK (modified Aschebrock and Kümmel meta-GGA functional), and LMBJ (local modified Becke-Johnson) exchange-correlation functionals. Our results strongly suggest that these meta-GGA functionals for supercell calculations perform quite well, especially, when compared to computationally more demanding GW calculations. We also present band offsets calculated using ionization potentials and electron affinities, as well as band alignment via the branch point energies. Overall, our study shows that the aforementioned meta-GGA functionals can be used within the DFT framework to estimate the band offsets in semiconductor heterostructures with predictive accuracy.

cond-mat.mtrl-sci↗

arXiv2022

Bandgap of two-dimensional materials: Thorough assessment of modern exchange-correlation functionals

The density functional theory (DFT) approximations that are the most accurate for the calculation of band gap of bulk materials are hybrid functionals like HSE06, the MBJ potential, and the GLLB-SC potential. More recently, generalized gradient approximations (GGA), like HLE16, or meta-GGAs, like (m)TASK, have proven to be also quite accurate for the band gap. Here, the focus is on 2D materials and the goal is to provide a broad overview of the performance of DFT functionals by considering a large test set of 298 2D systems. The present work is an extension of our recent studies [Rauch et al., Phys. Rev. B 101, 245163 (2020) and Patra et al., J. Phys. Chem. C 125, 11206 (2021)]. Due to the lack of experimental results for the band gap of 2D systems, $G_{0}W_{0}$ results were taken as reference. It is shown that the GLLB-SC potential and mTASK functional provide the band gaps that are the closest to $G_{0}W_{0}$. Following closely, the local MBJ potential has a pretty good accuracy that is similar to the accuracy of the more expensive hybrid functional HSE06.

cond-mat.mtrl-sci↗

arXiv2021

DensityTool: A post-processing tool for space- and spin-resolved density of states from VASP

The knowledge of the local electronic structure of heterogeneous solid materials is crucial for understanding their electronic, magnetic, transport, optical, and other properties. VASP, one of the mostly used packages for density-functional calculations, provides local electronic structure either by projecting the electronic wave functions on atomic spheres, or as a band-decomposed partial charge density. Here, we present a simple tool which takes the partial charge density and the energy eigenvalues calculated by VASP as input and constructs local charge and spin densities. The new data provides a much better spatial resolution than the projection on the atomic spheres. It can be visualized directly in the real space e.g. with Vesta, or averaged along planes spanned by two of the lattice vectors of the periodic unit cell. The plane-averaged local (spin) density of states can be easily plotted e.g. as color-coded data using almost any plotting program. DensityTool can be applied to manipulate, visualize, and understand the local electronic structure of any system calculated with VASP. We expect it to be useful especially for researchers concerned with inhomogeneous systems, such as interfaces, defects, surfaces, adsorbed molecules, or hybrid inorganic-organic composites.

cond-mat.mtrl-sci↗

arXiv2021

Electronic Structure and Epitaxy of CdTe Shells on InSb Nanowires

Indium antimonide (InSb) nanowires are used as building blocks for quantum devices because of their unique properties, i.e., strong spin-orbit interaction and large Landé g-factor. Integrating InSb nanowires with other materials could potentially unfold novel devices with distinctive functionality. A prominent example is the combination of InSb nanowires with superconductors for the emerging topological particles research. Here, we combine the II-VI cadmium telluride (CdTe) with the III-V InSb in the form of core-shell (InSb-CdTe) nanowires and explore potential applications based on the electronic structure of the InSb-CdTe interface and the epitaxy of CdTe on the InSb nanowires. We determine the electronic structure of the InSb-CdTe interface using density functional theory and extract a type-I band alignment with a small conduction band offset ($\leq$ 0.3 eV). These results indicate the potential application of these shells for surface passivation or as tunnel barriers in combination with superconductors. In terms of the structural quality of these shells, we demonstrate that the lattice-matched CdTe can be grown epitaxially on the InSb nanowires without interfacial strain or defects. These epitaxial shells do not introduce disorder to the InSb nanowires as indicated by the comparable field-effect mobility we measure for both uncapped and CdTe-capped nanowires.

cond-mat.mtrl-sci↗

arXiv2021

Local spin Hall conductivity

The spin Hall conductivity is usually calculated for periodic solids, while the knowledge of local contributions from inhomogeneous regions like interfaces or surfaces would be desirable. In this work we derive a local expression for the spin Hall conductivity of two-dimensional systems in analogy to the local anomalous Hall conductivity discussed recently. Our approach is applicable to heterogeneous fully bounded systems and nanoribbons with both open and periodic boundary conditions.

cond-mat.mes-hall↗

arXiv2021

Mirror Chern numbers in the hybrid Wannier representation

The topology of electronic states in band insulators with mirror symmetry can be classified in two different ways. One is in terms of the mirror Chern number, an integer that counts the number of protected Dirac cones in the Brillouin zone of high-symmetry surfaces. The other is via a $\mathbb{Z}_2$ index that distinguishes between systems that have a nonzero quantized orbital magnetoelectric coupling ("axion-odd"), and those that do not ("axion-even"); this classification can also be induced by other symmetries in the magnetic point group, including time reversal and inversion. A systematic characterization of the axion $\mathbb{Z}_2$ topology has previously been obtained by representing the valence states in terms of hybrid Wannier functions localized along one chosen crystallographic direction, and inspecting the associated Wannier band structure. Here we focus on mirror symmetry, and extend that characterization to the mirror Chern number. We choose the direction orthogonal to the mirror plane as the Wannierization direction, and show that the mirror Chern number can be determined from the winding numbers of the touching points between Wannier bands on mirror-invariant planes, and from the Chern numbers of flat bands pinned to those planes. In this representation, the relation between the mirror Chern number and the axion $\mathbb{Z}_2$ index is readily established. The formalism is illustrated by means of $\textit{ab initio}$ calculations for SnTe in the monolayer and bulk forms, complemented by tight-binding calculations for a toy model.

cond-mat.mes-hall↗

arXiv2020

Gapless hinge states from adiabatic pumping of axion coupling

We demonstrate that chiral hinge modes naturally emerge in insulating crystals undergoing a slow cyclic evolution that changes the Chern-Simons axion angle $θ$ by $2π$. This happens when the surface (not just the bulk) returns to its initial state at the end of the cycle, in which case it must pass through a metallic state to dispose of the excess quantum of surface anomalous Hall conductivity pumped from the bulk. If two adjacent surfaces become metallic at different points along the cycle, there is an interval in which they are in topologically distinct insulating states, with chiral modes propagating along the connecting hinge. We illustrate these ideas for a tight-binding model consisting of coupled layers of the Haldane model with alternating parameters. The surface topology is determined in a slab geometry using two different markers, surface anomalous Hall conductivity and surface-localized charge pumping (flow of surface-localized Wannier bands), and we find that both correctly predict the appearance of gapless hinge modes in a rod geometry. When viewing the axion pump as a four-dimensional (4D) crystal with one synthetic dimension, the hinge modes trace Fermi arcs in the Brillouin zone of the 2D hinge connecting a pair of 3D surfaces of the 4D crystal.

cond-mat.mtrl-sci↗

arXiv2020

Accurate electronic band gaps of two-dimensional materials from the local modified Becke-Johnson potential

The electronic band structures of two-dimensional materials are significantly different from those of their bulk counterparts, due to quantum confinement and strong modifications of electronic screening. An accurate determination of electronic states is a prerequisite to design electronic or optoelectronic applications of two-dimensional materials, however, most of the theoretical methods we have available to compute band gaps are either inaccurate, computationally expensive, or only applicable to bulk systems. Here we show that reliable band structures of nanostructured systems can now be efficiently calculated using density-functional theory with the local modified Becke-Johnson exchange-correlation functional that we recently proposed. After re-optimizing the parameters of this functional specifically for two-dimensional materials, we show, for a test set of almost 300 systems, that the obtained band gaps are of comparable quality as those obtained using the best hybrid functionals, but at a very reduced computational cost. These results open the way for accurate high-throughput studies of band-structures of two-dimensional materials and for the study of van der Waals heterostructures with large unit cells.

cond-mat.mes-hall↗

arXiv2020

Local modified Becke-Johnson exchange-correlation potential for interfaces, surfaces, and two-dimensional materials

The modified Becke-Johnson meta-GGA potential of density functional theory has been shown to be the best exchange-correlation potential to determine band gaps of crystalline solids. However, it cannot be consistently used for the electronic structure of non-periodic or nanostructured systems. We propose an extension of this potential that enables its use to study heterogeneous, finite and low-dimensional systems. This is achieved by using a coordinate-dependent expression for the parameter $c$ that weights the Becke-Russel exchange, in contrast to the original global formulation, where $c$ is just a fitted number. Our potential takes advantage of the excellent description of band gaps provided by the modified Becke-Johnson potential and preserves its modest computational effort. Furthermore, it yields with one single calculation band diagrams and band offsets of heterostructures and surfaces. We exemplify the usefulness and efficiency of our local meta-GGA potential by testing it for a series of interfaces (Si/SiO$_2$, AlAs/GaAs, AlP/GaP, and GaP/Si), a Si surface, and boron nitride monolayer.

cond-mat.mes-hall↗

arXiv2019

Non-trivial topological valence bands of common diamond and zinc-blende semiconductors

The diamond and zinc-blende semiconductors are well-known and have been widely studied for decades. Yet, their electronic structure still surprises with unexpected topological properties of the valence bands. In this joint theoretical and experimental investigation we demonstrate for the benchmark compounds InSb and GaAs that the electronic structure features topological surface states below the Fermi energy. Our parity analysis shows that the spin-orbit split-off band near the valence band maximum exhibits a strong topologically non-trivial behavior characterized by the $\mathcal{Z}_2$ invariants $(1;000)$. The non-trivial character emerges instantaneously with non-zero spin-orbit coupling, in contrast to the conventional topological phase transition mechanism. \textit{Ab initio}-based tight-binding calculations resolve topological surface states in the occupied electronic structure of InSb and GaAs, further confirmed experimentally by soft X-ray angle-resolved photoemission from both materials. Our findings are valid for all other materials whose valence bands are adiabatically linked to those of InSb, i.e., many diamond and zinc-blende semiconductors, as well as other related materials, such as half-Heusler compounds.

cond-mat.mtrl-sci↗

arXiv2018

Geometric and nongeometric contributions to the surface anomalous Hall conductivity

A static electric field generates circulating currents at the surfaces of a magnetoelectric insulator. The anomalous Hall part of the surface conductivity tensor describing such bound currents can change by multiples of $e^2/h$ depending on the insulating surface preparation, and a bulk calculation does not fix its quantized part. To resolve this ambiguity, we develop a formalism for calculating the full surface anomalous Hall conductivity in a slab geometry. We identify a Berry-curvature term, closely related to the expression for the bulk anomalous Hall conductivity, whose value can change by quantized amounts by adjusting the surface Hamiltonian. In addition, the surface anomalous Hall conductivity contains a nongeometric part that does not depend on the surface preparation.

cond-mat.mes-hall↗

arXiv2017

Double Band Inversion in $ α$-Sn: Appearance of Topological Surface States and the Role of Orbital Composition

The electronic structure of \graySn(001) thin films strained compressively in-plane was studied both experimentally and theoretically. A new topological surface state (TSS) located entirely within the gapless projected bulk bands is revealed by \textit{ab initio}-based tight-binding calculations as well as directly accessed by soft X-ray angle-resolved photoemission. The topological character of this state, which is a surface resonance, is confirmed by unravelling the band inversion and by calculating the topological invariants. In agreement with experiment, electronic structure calculations show the maximum density of states in the subsurface region, while the already established TSS near the Fermi level is strongly localized at the surface. Such varied behavior is explained by the differences in orbital composition between the specific TSS and its associated bulk states, respectively. This provides an orbital protection mechanism for topological states against mixing with the background of bulk bands.

cond-mat.str-el↗

arXiv2016

Topological Crystalline Transition Metals: Strained W, Ta, Mo, and Nb

In a joint theoretical and experimental investigation we show that a series of transition metals with strained body-centered cubic lattice ---W, Ta, Nb, and Mo--- host surface states that are topologically protected by mirror symmetry. Our finding extends the class of topologically nontrivial systems by topological crystalline transition metals. The investigation is based on independent calculations of the electronic structures and of topological invariants, the results of which agree with established properties of the Dirac-type surface state in W(110). To further support our prediction, we investigate both experimentally by spin-resolved inverse photoemission and theoretically an unoccupied topologically nontrivial surface state in Ta(110).

cond-mat.mtrl-sci↗

arXiv2015

Impact of the Topological Surface State on the Thermoelectric Transport in Sb$_2$Te$_3$ Thin Films

Ab initio electronic structure calculations based on density functional theory and tight-binding methods for the thermoelectric properties of p-type Sb$_2$Te$_3$ films are presented. The thickness-dependent electrical conductivity and the ther- mopower are computed in the diffusive limit of transport based on the Boltzmann equation. Contributions of the bulk and the surface to the transport coefficients are separated which enables to identify a clear impact of the topological surface state on the thermoelectric properties. By tuning the charge carrier concentration, a crossover between a surface-state-dominant and a Fuchs-Sondheimer transport regime is achieved. The calculations are corroborated by thermoelectric transport measurements on Sb$_2$Te$_3$ films grown by atomic layer deposition.

cond-mat.mtrl-sci↗