arXiv subjects

Qihang Liu

Publications and source records attributed to Qihang Liu.

At least 91 records · Page 5Linked to original sources

arXiv2019

Rational design principles of quantum anomalous Hall effect from superlattice-like magnetic topological insulators

As one of paradigmatic phenomena in condensed matter physics, the quantum anomalous Hall effect (QAHE) in stoichiometric Chern insulators has drawn great interest for years. By using model Hamiltonian analysis and first-principle calculations, we establish a topological phase diagram and map on it with different two-dimensional configurations, which is taken from the recently-grown magnetic topological insulators MnBi4Te7 and MnBi6Te10 with superlattice-like stacking patterns. These configurations manifest various topological phases, including quantum spin Hall effect with and without time-reversal symmetry, as well as QAHE. We then provide design principles to trigger QAHE by tuning experimentally accessible knobs, such as slab thickness and magnetization. Our work reveals that superlattice-like magnetic topological insulators with tunable exchange interaction serve as an ideal platform to realize the long-sought QAHE in pristine compounds, paving a new avenue within the area of topological materials.

cond-mat.mes-hall↗

arXiv2019

Dimensional crossover and topological nature of the thin films of a three-dimensional topological insulator by band gap engineering

Identification and control of topological phases in topological thin films offer great opportunity for fundamental research and the fabrication of topology-based devices. Here, combining molecular beam epitaxy, angle-resolved photoemission spectroscopy and ab-initio calculations, we investigate the electronic structure evolution in (Bi1-xInx)2Se3 films with thickness from 2 to 13 quintuple layers. We identify several phases with their characteristic topological nature and evolution between them, i.e., dimensional crossover from a three-dimensional topological insulator with gapless surface state to its two-dimensional counterpart with gapped surface state, and topological phase transition from topological insulator to a normal semiconductor with increasing In concentration x. Furthermore, by introducing In alloying as an external knob of band gap engineering, we experimentally demonstrated the trivial topological nature of Bi2Se3 thin films (below 6 quintuple layers) as two-dimensional gapped systems, in consistent with our theoretical calculations. Our results provide not only a comprehensive phase diagram of (Bi1-xInx)2Se3 and a route to control its phase evolution, but also a practical way to experimentally determine the topological properties of a gapped compound by topological phase transition and band gap engineering.

cond-mat.mtrl-sci↗

arXiv2019

Disorder-Induced Weyl Semimetal Phase and Sequential Band Inversions in PbSe-SnSe Alloys

The search for topological systems has recently broadened to include random substitutional alloys, which lack the specific crystalline symmetries that protect topological phases, raising the question whether topological properties can be preserved, or are modified by disorder. To address this question, we avoid methods that assumed at the outset high (averaged) symmetry, using instead a fully-atomistic, topological description of alloy. Application to PbSe-SnSe alloy reveals that topology survives in an interesting fashion: (a) spatial randomness removes the valley degeneracy (splitting larger than 150 meV), leading to a sequential inversion of the split valley components over a range of compositions; (b) absence of inversion lifts spin degenerates, leading to a Weyl semimetal phase without the need of external magnetic field, an unexpected result, given that the alloy constituent compounds are inversion-symmetric. (a) and (b) underpin the topological physics at low symmetry and complete the missing understanding of possible topological phases within the normal-topological insulator transition.

cond-mat.mtrl-sci↗

arXiv2019

Symmetry-assisted protection and compensation of hidden spin polarization in centrosymmetric systems

It is recently noted that in certain centrosymmetric compounds, spin-orbit interaction couples each local sector that lacks inversion symmetry and thus leads to visible spin polarization effects in the real space, dubbed as 'hidden spin polarization (HSP)'. However, observable spin polarization of a given local sector suffers interference by its inversion partner, impeding material realization and potential applications of HSP. Starting from a single-orbital tight-binding model, we propose a nontrivial way to protect strong sector-projected spin texture through minimizing the interaction between inversion partners by nonsymmorphic symmetry. The HSP effect is generally compensated by inversion partners near the Γ point but immune from interaction around the boundary of the Brillouin zone. We further summarize 17 layer groups that support such symmetry-assisted HSP and identify by first-principle calculations hundreds of quasi-2D materials from the existing databases, among which a group of rare-earth compounds LnOI (Ln = Pr, Nd, Ho, Tm and Lu) serves as great candidates showing strong Rashba- and Dresselhaus-type HSP. Our finding also provides an ideal platform to control HSP for emergent physical effects, such as opening a hybridization gap by tensile strain to realize the time-reversal-invariant topological superconductivity.

cond-mat.mes-hall↗

arXiv2019

Anti-doping in Insulators and Semiconductors having Intermediate Bands with Trapped Carriers

Ordinary doping by electrons (holes) generally means that the Fermi level shifts towards the conduction band (valence band) and that the conductivity of free carriers increases. Recently, however, some peculiar doping characteristics were sporadically recorded in different materials without noting the mechanism: electron doping was observed to cause a portion of the lowest unoccupied band to merge into the valance band, leading to a decrease in conductivity. This behavior we dub as 'anti-doping' was seen in rare-earth nickel oxides SmNiO3, cobalt oxides SrCoO2.5, Li-ion battery materials and even MgO with metal vacancies. We describe the physical origin of anti-doping as well as its inverse problem, the 'design principles' that would enable intelligent search of materials. We find that electron anti-doping is expected in materials having pre-existing trapped holes and is caused by annihilation of such 'hole polarons' via electron doping. This may offer an unconventional way of controlling conductivity.

cond-mat.mtrl-sci↗

arXiv2018

Uncovering and tailoring hidden Rashba spin-orbit splitting in centrosymmetric crystals

Hidden Rashba and Dresselhaus spin-splittings in centrosymmetric crystals with subunits (sectors) having non-centrosymmetric symmetries (the R-2 and D-2 effects) have been predicted and observed experimentally, but the microscopic mechanism remains unclear. Here we demonstrate that the spin-splitting in R-2 is enforced by specific symmetries (such as the non-symmorphic in the present example) which ensures that the pertinent spin wavefunctions segregate spatially on just one of the two inversion-partner sectors and thus avoid compensation. This finding establishes a common fundamental source for the conventional Rashba (R-1) effect and the R-2 effect, both originating from the local sector symmetries, rather than from the global crystal asymmetry alone for R-1 per se. We further show that the effective Hamiltonian for the R-1 effect is also applicable for the R-2 effect, but applying a symmetry-breaking electric field to an R-2 compound produces different spin-splitting pattern than applying a field to a trivial (non-R-2) centrosymmetric compound.

cond-mat.mtrl-sci↗

arXiv2018

Bond disproportionation, charge self-regulation and ligand holes in s-p and in d electron ABX3 perovskites by density functional theory

Some ABX3 perovskites exhibit different local environments (DLE) for the same B atoms in the lattice, an effect referred to as disproportionation, distinguishing such compounds from perovskites that have single local environments (SLE). The basic phenomenology of disproportionation involves the absence of B-atom charge ordering, the creation of different B-X bond length for different local environments, the appearance of metal (in SLE) to insulator (in DLE) transition, and the formation of ligand holes. We point out that this phenomenology is common to a broad range of chemical bonding patterns in ABX3 compounds, either with s-p electron B-metal cations (BaBiO3, CsTlF3), or noble metal cation (CsAuCl3), as well as d-electron cations (SmNiO3, CaFeO3). We show that underlying much of this phenomenology is the self-regulating response, whereby in strongly bonded metal-ligand systems with high lying ligand orbitals, the system protects itself from creating highly charged cations by transferring ligand electrons to the metal, thus preserving a nearly constant metal charge in DLE, while creating B-ligand bond alternation and ligand-like conduction band (ligand hole). We are asking what are the minimal theory ingredients needed to explain the main features of this SLE-to-DLE phenomenology, such as its energetic driving force, bond length changes, possible modifications in charge density and density of state changes. Using as a guide the lowering of the total energy in DLE relative to SLE, we show that density functional calculations describe this phenomenology across the whole chemical bonding range without resort to special strong correlation effects, beyond what DFT naturally contains. In particular, lower total energy configurations (DLE) naturally develop bond alternation, gaping of the metallic SLE state, and absence of charge ordering with ligand hole formation.

cond-mat.mtrl-sci↗

arXiv2018

Topological insulators vs. topological Dirac semimetals in honeycomb compounds

Intriguing physical property of materials stems from their chemical constituent whereas the connection between them is often not clear. Here, we uncover a general chemical classification for the two quantum phases in the honeycomb ABX structure--topological insulator (TI) and topological Dirac semimetal (TDSM). First, we find among the 816 (existing as well as hypothetical) calculated compounds, 160 TI's (none were noted before), 96 TDSM's, 282 normal insulators (NI's), and 278 metals. Second, based on this classification, we have distilled a simple chemical regularity based on compound formulae for the selectivity between TI and TDSM: The ABX compounds that are TDSM have B atoms (part of the BX honeycomb layers) that come from the Periodic Table columns XI (Cu, Ag, Au) or XII (Zn, Cd, Hg), or Mg (group II), whereas the ABX compounds whose B atoms come from columns I (Li, Na, K, Rb, Cs) or II (Ca, Sr, Ba) are TI's. Third, focusing on the ABX Bismide compounds that are thermodynamically stable, we find a structural motif that delivers topological insulation and stability at the same time. This study opens the way to simultaneously design new topological materials based on the compositional rules indicated here.

cond-mat.mtrl-sci↗

arXiv2018

Electron doping of proposed quantum spin liquid kagomé Zn-Cu hydroxyl-halides produces localized states in the band gap

Carrier doping of quantum spin liquids is a long-proposed route to the emergence of high-temperature superconductivity. Electrochemical intercalation in kagome hydroxyl-halide materials shows that samples remain insulating across a wide range of electron counts. Here we demonstrate through first-principles density functional calculations corrected for self-interaction the mechanism by which electrons remain localized in various Zn-Cu hydroxyl-halides, independently of the chemical identity of the dopant - the formation of polaronic states with attendant lattice displacements and a dramatic narrowing of bandwidth upon electron addition. The same theoretical method applied to electron doping in cuprate Nd2CuO4 correctly produces a metallic state when the initially formed polaron dissolves into an extended state. Our general findings explain the insulating behavior in a wide range of doped quantum magnets and demonstrate that new quantum spin liquid host materials are needed to realize metallicity borne of a spin liquid.

cond-mat.mtrl-sci↗

arXiv2017

Coexistence of Tunable Weyl Points and Topological Nodal Lines in Ternary Transition-Metal Telluride TaIrTe4

We report a combined theoretical and experimental study on TaIrTe4, a potential candidate of the minimal model of type-II Weyl semimetals. Unexpectedly, an intriguing node structure with twelve Weyl points and a pair of nodal lines protected by mirror symmetry was found by first-principle calculations, with its complex signatures such as the topologically non-trivial band crossings and topologically trivial Fermi arcs cross-validated by angle-resolved photoemission spectroscopy. Through external strain, the number of Weyl points can be reduced to the theoretical minimum of four, and the appearance of the nodal lines can be switched between different mirror planes in momentum space. The coexistence of tunable Weyl points and nodal lines establishes ternary transition-metal tellurides as a unique test ground for topological state characterization and engineering.

cond-mat.mtrl-sci↗

arXiv2017

Changes in charge density vs changes in formal oxidation states: The case of Sn halide perovskites and their ordered vacancy analogues

Shifting the Fermi energy in solids by doping, defect formation or gating generally results in changes in the charge density distribution, which reflect the ability of the bonding pattern in solids to adjust to such external perturbations. In the ionic limit, such changes are described by the formal oxidation states (FOS) whereby a single atom type is presumed to absorb the full burden of the perturbation (change in charge) of the whole compound. In this picture, when the solar absorber CsSnI3 loses 50 % of its Sn atoms thereby forming the ordered vacancy compound Cs2SnI6, the Sn is said to change from Sn2+ to Sn4+. In reality, the charge redistribution is more complex. To understand the electronic properties of these two groups and to gauge the trends in s-electron charge on the nucleus, we studied the 113/216 compound pairs CsSnCl3/Cs2SnCl6; CsSnBr3/Cs2SnBr6, and CsSnI3/Cs2SnI6. We have calculated the electronic structure of these three compound pairs, complementing them by CsSnF3/Cs2SnF6 in the hypothetical cubic structure for completing the chemical trends. These materials were also synthesized by chemical routes and characterized by X-ray diffraction, Mossbauer spectroscopy and K-edge X-ray Absorption Spectroscopy. We find that in going from 113 to 216 there is a decrease in the s charge on Sn, in agreement with the FOS picture. However, at the same time, we observe an increase of the p charge via downshift of the otherwise unoccupied p level, an effect that tends to replenish much of the lost s charge. This effect is theoretically explained as a self-regulating response [H. Raebiger, S. Lany, and A. Zunger, Nature 453, 763 (2008)] whereby the system re-hybridizes to minimize the effect of the charge perturbation created by vacancy formation. Our work clarifies the relation between FOS and charge transfer that can be applied to a wide variety of materials.

cond-mat.mtrl-sci↗

arXiv2017

Predicted Realization of Cubic Dirac Fermion in Quasi-One-Dimensional Transition-Metal MonoChalcogenides

We show that the previously predicted Fermion particle that has no analogue in the standard model of particle theory - the cubically dispersed Dirac semimetal (CDSM) - is realized in a specific, stable solid state system that has been made years ago, but was not appreciated to host such a unique Fermion, composed of six Weyl Fermions, 3 with left-handed and 3 with right-handed chirality. We identified the crystal symmetry constraints and found the space group P63/m as one of the two that can support a CDSM, of which the characteristic band crossing has linear dispersion along the principle axis but cubic dispersion in the plane perpendicular to it. We then conducted a material search using density functional theory identifying a group of quasi-one-dimensional molybdenum mono-chalcogenide compounds A(MoX)3 (A = Na, K, Rb, In, Tl, X = S, Se, Te) as ideal CDSM candidates. Studying the stability of the A(MoX)3 family reveals a few candidates such as Rb(MoTe)3 and Tl(MoTe)3 that are predicted to be resilient to Peierls distortion, thus retaining the metallic character. The combination of one-dimensionality and metallic nature in this family provides a platform for unusual optical signature - polarization dependent metallic vs insulating response.

cond-mat.mtrl-sci↗

arXiv2017

The enabling electronic motif for topological insulation in ABO3 perovskites and its structural stability

Stable oxide topological insulators (TIs) that could bring together the traditional oxide functionalities with the dissipationless surface states of TIs have been sought for years but none was found. Yet, heavier chalcogenides (selenides, tellurides) were readily found to be TIs. We clarify here the basic contradiction between TI-ness and stability which is maximal for oxides, and trace the basic design principles necessary to identify the window of opportunity of stable TIs. We first identify the electronic motif that can achieve topological band inversion ("topological gene") in ABO3 as being a lone-pair electron-rich B atom (e.g. Te, I, Bi) at the octahedral site. We then illustrate that poorly screened oxide systems with large inversion energies can undergo energy-lowering atomic distortions that remove the band inversion. We identify the coexistence windows of TI functionality and structure stability for different pressures and find that the common cubic ABO3 structures have inversion energies lying outside this coexistence window at zero pressure but could be moved into the coexistence window at moderate pressures. Our study demonstrates the interplay between topological band inversion and structural stability and traces the basic principles needed to design stable oxide topological insulators at ambient pressures.

cond-mat.mtrl-sci↗

arXiv2017

Predicted electronic markers for polytypes of LaOBiS2 examined via angular resolved photoemission spectroscopy

The natural periodic stacking of symmetry-inequivalent planes in layered compounds can lead to the formation of natural superlattices; albeit close in total energy, (thus in their thermodynamic stability), such polytype superlattices can exhibit different structural symmetries, thus have markedly different electronic properties which can in turn be used as "structural markers". We illustrate this general principle on the layered LaOBiS2 compound where density-functional theory (DFT) calculations on the (BiS2)/(LaO)/(BiS2) polytype superlattices reveal both qualitatively and quantitatively distinct electronic structure markers associated with the Rashba physics, yet the total energies are only ~ 0.1 meV apart. This opens the exciting possibility of identifying subtle structural features via electronic markers. We show that the pattern of removal of band degeneracies in different polytypes by the different forms of symmetry breaking leads to new Rashba "mini gaps" with characteristic Rashba parameters that can be determined from spectroscopy, thereby narrowing down the physically possible polytypes. By identifying these distinct DFT-predicted fingerprints via ARPES measurements on LaBiOS2 we found the dominant polytype with small amounts of mixtures of other polytypes. This conclusion, consistent with neutron scattering results, establishes ARPES detection of theoretically established electronic markers as a powerful tool to delineate energetically quasidegenerate polytypes.

cond-mat.mtrl-sci↗

arXiv2016

Minimal Ingredients for Orbital Texture Switches at Dirac Points in Strong Spin-Orbit Coupled Materials

Recent angle resolved photoemission spectroscopy measurements on strong spin-orbit coupled materials have shown an in-plane orbital texture switch at their respective Dirac points, regardless of whether they are topological insulators or "trivial" Rashba materials. This feature has also been demonstrated in a few materials ($\text{Bi}_2\text{Se}_3$, $\text{Bi}_2\text{Te}_3$, and $\text{BiTeI}$) though DFT calculations. Here we present a minimal orbital-derived tight binding model to calculate the electron wave-function in a two-dimensional crystal lattice. We show that the orbital components of the wave-function demonstrate an orbital-texture switch in addition to the usual spin switch seen in spin polarized bands. This orbital texture switch is determined by the existence of three main properties: local or global inversion symmetry breaking, strong spin-orbit coupling, and non-local physics (the electrons are on a lattice). Using our model we demonstrate that the orbital texture switch is ubiquitous and to be expected in many real systems. The orbital hybridization of the bands is the key aspect for understanding the unique wave function properties of these materials, and this minimal model helps to establish the quantum perturbations that drive these hybridizations.

cond-mat.mtrl-sci↗

arXiv2016

Orbital mapping of energy bands and the truncated spin polarization in three-dimensional Rashba semiconductors

Associated with spin-orbit coupling (SOC) and inversion symmetry breaking, Rashba spin polarization opens a new avenue for spintronic applications that was previously limited to ordinary magnets. However, spin polarization effects in actual Rashba systems are far more complicated than what conventional single-orbital models would suggest. By studying via first-principles DFT and a multi-orbital k.p model a 3D bulk Rashba system (free of complications by surface effects) we find that the physical origin of the leading spin polarization effects is SOC-induced hybridization between spin and multiple orbitals, especially those with nonzero orbital angular momenta. In this framework we establish a general understanding of the orbital mapping, common to the surface of topological insulators and Rashba system. Consequently, the intrinsic mechanism of various spin polarization effects, which pertain to all Rashba systems even those with global inversion symmetry, is understood as a manifestation of the orbital textures. This finding suggests a route for designing high spin-polarization materials by considering the atomic-orbital content.

physics.comp-ph↗

arXiv2016

Polytypism in LaOBiS2-type compounds based on different three-dimensional stacking sequences of two-dimensional BiS2 layers

LaOBiS2-type materials have drawn much attention recently because of various interesting physical properties, such as low-temperature superconductivity, hidden spin polarization, and electrically tunable Dirac cones. However, it was generally assumed that each LaOBiS2-type compound has a unique and specific crystallographic structure (with a space group P4/nmm) separated from other phases. Using first-principles total energy and stability calculations we confirm that the previous assignment of the centrosymetric P4/nmm structure to LaOBiS2 is incorrect as a phonon instability renders this structure impossible. Furthermore, we find that the unstable structure is replaced by a family of energetically closely spaced modifications (polytypes) differing by the layer sequences and orientations. We find that the local Bi-S distortion leads to three polytypes of LaOBiS2 with different stacking patterns of the distorted BiS2 layers. The energy difference between the polytypes of LaOBiS2 is merely ~1 meV/u.c., indicating the possible coexistence of all polytypes in the real sample and that the particular distribution of polytypes may be growth-induced. The in-plane distortion can be suppressed by pressure, leading to a phase transition from polytypes to the high-symmetry P4/nmm structure with a pressure larger than 2.5 GPa. In addition, different choices of the intermediate atoms (replacing La) or active atoms (BiS2) could also manifest different ground state structures. One can thus tune the distortion and the ground state by pressure or substituting covalence atoms in LaOBiS2-family.

cond-mat.mtrl-sci↗

arXiv2016

Transforming common III-V and II-VI semiconductor compounds into topological heterostructures: The case of CdTe/InSb superlattices

Currently known topological insulators (TIs) are limited to narrow gap compounds incorporating heavy elements, thus severely limiting the material pool available for such applications. We show via first-principle calculations how a heterovalent superlattice made of common semiconductor building blocks can transform its non-TI components into a topological nanostructure, illustrated by III-V/II-VI superlattice InSb/CdTe. The heterovalent nature of such interfaces sets up, in the absence of interfacial atomic exchange, a natural internal electric field that along with the quantum confinement leads to band inversion, transforming these semiconductors into a topological phase while also forming a giant Rashba spin splitting. We reveal the relationship between the interfacial stability and the topological transition, finding a window of opportunity where both conditions can be optimized. Once a critical InSb layer thickness above ~ 1.5 nm is reached, both [111] and [100] superlattices have a relative energy of 5-14 meV/A2 higher than that of the atomically exchanged interface and an excitation gap up to ~150 meV, affording room-temperature quantum spin Hall effect in semiconductor superlattices. The understanding gained from this study could significantly broaden the current, rather restricted repertoire of functionalities available from individual compounds by creating next-generation super-structured functional materials.

cond-mat.mtrl-sci↗