Publications

Due to quasi-one-dimensional confinement, nanowires possess unique electronic properties, which can promote specific device architectures. However, nanowire growth presents paramount challenges, limiting the accessible crystal structures and elemental compositions. Here we demonstrate solid-state topotactic exchange that converts wurtzite InAs nanowires into Zintl Eu₃In₂As₄. Molecular-beam-epitaxy-based in situ evaporation of Eu and As onto InAs nanowires results in the mutual exchange of Eu from the shell and In from the core. Therefore, a single-phase Eu₃In₂As₄ shell grows, which gradually consumes the InAs core. The mutual exchange is supported by the substructure of the As matrix, which is similar across the wurtzite InAs and Zintl Eu₃In₂As₄ and therefore is topotactic. The Eu₃In₂As₄ nanowires undergo an antiferromagnetic transition at a Néel temperature of ~6.5 K. Ab initio calculations confirm the antiferromagnetic ground state and classify Eu₃In₂As₄ as a C₂T axion insulator, hosting both chiral hinge modes and unpinned Dirac surface states. The topotactic mutual-exchange nanowire growth will, thus, enable the exploration of intricate magneto-topological states in Eu₃In₂As₄ and potentially in other exotic compounds.

Bi₂SeO₅ has garnered considerable attention as a van der Waals (vdW) layered dielectric material featuring excellent electrical insulation properties. However, the related theoretical understanding of the dielectric properties of atomically thin films is still lacking. Here, we conducted the first-principles calculations to determine the dielectric performance of Bi₂SeO₅, showing a high average dielectric constant (ε) of >20 ranging from bulk to bilayer and monolayer. Besides, the conduction and valance band offsets between the monolayer Bi₂SeO₅ and bilayer Bi₂O₂Se were calculated to be greater than 1 eV, suggesting that monolayer Bi₂SeO₅ works well as the dielectric for atomically thin Bi₂O₂Se. Unlike h-BN or other two-dimensional (2D) vdW insulators, ε of Bi₂SeO₅ is dominated by its ionic component and remains nearly constant as the thickness decreases, demonstrating an ultralow equivalent oxide thickness (EOT) of 0.3 nm for its monolayer form. Moreover, the high ε of monolayer Bi₂SeO₅ survives under tensile or compressive strains up to 6%, which greatly facilitates its integration with various 2D semiconductors. Our work suggests that Bi₂SeO₅ ultrathin films can serve as excellent atomically flat encapsulation and dielectric layers for high-performance 2D electronic devices.[Figure not available: see fulltext.]

Controlling and understanding electron correlations in quantum matter is one of the most challenging tasks in materials engineering. In the past years a plethora of new puzzling correlated states have been found by carefully stacking and twisting two-dimensional van der Waals materials of different kind. Unique to these stacked structures is the emergence of correlated phases not foreseeable from the single layers alone. In Ta-dichalcogenide heterostructures made of a good metallic \u201c1H\u201d- and a Mott insulating \u201c1T\u201d-layer, recent reports have evidenced a cross-breed itinerant and localized nature of the electronic excitations, similar to what is typically found in heavy fermion systems. Here, we put forward a new interpretation based on first-principles calculations which indicates a sizeable charge transfer of electrons (0.4-0.6 e) from 1T to 1H layers at an elevated interlayer distance. We accurately quantify the strength of the interlayer hybridization which allows us to unambiguously determine that the system is much closer to a doped Mott insulator than to a heavy fermion scenario. Ta-based heterolayers provide therefore a new ground for quantum-materials engineering in the regime of heavily doped Mott insulators hybridized with metallic states at a van der Waals distance.

Quantum oscillations originating from the quantization of electron cyclotron orbits provide sensitive diagnostics of electron bands and interactions. We report on nanoscale imaging of the thermodynamic magnetization oscillations caused by the de Haas-van Alphen effect in moiré graphene. Scanning by means of superconducting quantum interference device (SQUID)-on-tip in Bernal bilayer graphene crystal axis-aligned to hexagonal boron nitride reveals large magnetization oscillations with amplitudes reaching 500 Bohr magneton per electron in weak magnetic fields, unexpectedly low frequencies, and high sensitivity to superlattice filling fraction. The oscillations allow us to reconstruct the complex band structure, revealing narrow moiré bands with multiple overlapping Fermi surfaces separated by unusually small momentum gaps. We identified sets of oscillations that violate the textbook Onsager Fermi surface sum rule, signaling formation of broad-band particle-hole superposition states induced by coherent magnetic breakdown.

The ability to selectively excite light with fixed handedness is crucial for circularly polarized light emission. It is commonly believed that the luminescent material chirality determines the emitted light handedness, regardless of the light emitting direction. In this paper, we propose an anomalous circular polarized light emission (ACPLE) whose handedness actually relies on the emission direction and current direction in electroluminescence. In a solid semiconductor, the ACPLE originates in the band structure topology characterized by the optical Berry curvature dipole. ACPLE exists in inversion-symmetry breaking materials including chiral materials. We exemplify the ACPLE by estimating the high circular polarization ratio in monolayer WS2. In addition, the ACPLE can be further generalized to magnetic semiconductors in which the optical Berry curvature plays a leading role instead. Our finding reveals intriguing consequences of band topology in light emission and promises optoelectric applications.

The interplay between chirality and topology nurtures many exotic electronic properties. For instance, topological chiral semimetals display multifold chiral fermions that manifest nontrivial topological charge and spin texture. They are an ideal playground for exploring chirality-driven exotic physical phenomena. In this work, we reveal a monopole-like orbital-momentum locking texture on the three-dimensional Fermi surfaces of topological chiral semimetals with B20 structures (e.g., RhSi and PdGa). This orbital texture enables a large orbital Hall effect (OHE) and a giant orbital magnetoelectric (OME) effect in the presence of current flow. Different enantiomers exhibit the same OHE which can be converted to the spin Hall effect by spin-orbit coupling in materials. In contrast, the OME effect is chirality-dependent and much larger than its spin counterpart. Our work reveals the crucial role of orbital texture for understanding OHE and OME effects in topological chiral semimetals and paves the path for applications in orbitronics, spintronics, and enantiomer recognition.

Layered crystalline materials that consist of transition metal atoms on a kagome network have emerged as a versatile platform for the study of unusual electronic phenomena. For example, in the vanadium-based kagome superconductors AV₃Sb₅ (where A can stand for K, Cs or Rb), there is a parent charge density wave phase that appears to simultaneously break both the translational and rotational symmetries of the lattice. Here we show a contrasting situation, where electronic nematic order\u2014the breaking of rotational symmetry without the breaking of translational symmetry\u2014can occur without a corresponding charge density wave. We use spectroscopic-imaging scanning tunnelling microscopy to study the kagome metal CsTi₃Bi₅ that is isostructural to AV₃Sb₅ but with a titanium atom kagome network. CsTi₃Bi₅ does not exhibit any detectable charge density wave state, but a comparison to density functional theory calculations reveals substantial electronic correlation effects at low energies. In comparing the amplitudes of scattering wave vectors along different directions, we discover an electronic anisotropy that breaks the sixfold symmetry of the lattice, arising from both in-plane and out-of-plane titanium-derived d orbitals. Our work uncovers the role of electronic orbitals in CsTi₃Bi₅, suggestive of a hexagonal analogue of the nematic bond order in Fe-based superconductors.

Strong singularities in the electronic density of states amplify correlation effects and play a key role in determining the ordering instabilities in various materials. Recently high order van Hove singularities (VHSs) with diverging power-law scaling have been classified in single-band electron models. We show that the 110 surface of Bismuth exhibits high order VHS with an usually high density of states divergence ∼ (E)^−0.7. Detailed mapping of the surface band structure using scanning tunneling microscopy and spectroscopy combined with first-principles calculations show that this singularity occurs in close proximity to Dirac bands located at the center of the surface Brillouin zone. The enhanced power-law divergence is shown to originate from the anisotropic flattening of the Dirac band just above the Dirac node. Such near-coexistence of massless Dirac electrons and ultra-massive saddle points enables to study the interplay of high order VHS and Dirac fermions.

Hysteretic switching of domain states is a salient characteristic of all ferroic materials and the foundation for their multifunctional applications. Ferro-rotational order is emerging as a type of ferroic order that features structural rotations, but control over state switching remains elusive due to its invariance under both time reversal and spatial inversion. Here we demonstrate electrical switching of ferro-rotational domain states in the charge-density-wave phases of nanometre-thick 1T-TaS₂ crystals. Cooling from the high-symmetry phase to the ferro-rotational phase under an external electric field induces domain state switching and domain wall formation, which is realized in a simple two-terminal configuration using a volt-scale bias. Although the electric field does not couple with the order due to symmetry mismatch, it drives domain wall propagation to give rise to reversible, durable and non-volatile isothermal state switching at room temperature. These results offer a route to the manipulation of ferro-rotational order and its nanoelectronic applications.

The recently discovered kagome materials AV₃Sb₅ (A = K, Rb, Cs) attract intense research interest in intertwined topology, superconductivity, and charge density waves (CDW). Although the in-plane 2 × 2 CDW is well studied, its out-of-plane structural correlation with the Fermi surface properties is less understood. In this work, we advance the theoretical description of quantum oscillations and investigate the Fermi surface properties in the three-dimensional CDW phase of CsV₃Sb₅. We derived Fermi-energy-resolved and layer-resolved quantum orbits that agree quantitatively with recent experiments in the fundamental frequency, cyclotron mass, and topology. We reveal a complex Dirac nodal network that would lead to a π Berry phase of a quantum orbit in the spinless case. However, the phase shift of topological quantum orbits is contributed by the orbital moment and Zeeman effect besides the Berry phase in the presence of spin-orbital coupling (SOC). Therefore, we can observe topological quantum orbits with a π phase shift in otherwise trivial orbits without SOC, contrary to common perception. Our work reveals the rich topological nature of kagome materials and paves a path to resolve different topological origins of quantum orbits.

The scaling of silicon-based transistors at sub-ten-nanometre technology nodes faces challenges such as interface imperfection and gate current leakage for an ultrathin silicon channel^1,2. For next-generation nanoelectronics, high-mobility two-dimensional (2D) layered semiconductors with an atomic thickness and dangling-bond-free surfaces are expected as channel materials to achieve smaller channel sizes, less interfacial scattering and more efficient gate-field penetration^1,2. However, further progress towards 2D electronics is hindered by factors such as the lack of a high dielectric constant (κ) dielectric with an atomically flat and dangling-bond-free surface^3,4. Here, we report a facile synthesis of a single-crystalline high-κ (κ of roughly 16.5) van der Waals layered dielectric Bi₂SeO₅. The centimetre-scale single crystal of Bi₂SeO₅ can be efficiently exfoliated to an atomically flat nanosheet as large as 250 × 200 μm² and as thin as monolayer. With these Bi₂SeO₅ nanosheets as dielectric and encapsulation layers, 2D materials such as Bi₂O₂Se, MoS₂ and graphene show improved electronic performances. For example, in 2D Bi₂O₂Se, the quantum Hall effect is observed and the carrier mobility reaches 470,000 cm² V⁻¹ s⁻¹ at 1.8 K. Our finding expands the realm of dielectric and opens up a new possibility for lowering the gate voltage and power consumption in 2D electronics and integrated circuits.

The prevalent global energy crisis calls for searching viable pathways for generating green hydrogen as an alternative energy resource. Dye-sensitized photocatalytic water splitting is a feasible solution to produce green hydrogen. However, identifying suitable catalysts has been one of the bottlenecks in driving dye-sensitized photocatalysis efficiently. In this work, a new class of electrocatalysts is reported based on the layered Weyl semimetals MIrTe₄ (M = Nb, Ta) for the Eosin Y (EY)-sensitized hydrogen evolution reaction (HER). NbIrTe₄ and TaIrTe₄ exhibit HER activities of ≈18 000 and 14 000 µmol g⁻¹ respectively, after 10 h of irradiation with visible light. Time-dependent UV-Vis spectroscopy and high-pressure liquid chromatography coupled with mass spectrometry analysis shed light on the reaction dynamics and enable a deeper understanding of the observed trend in hydrogen evolution rates for MIrTe₄. MIrTe₄ semimetals outperform transition metal-based Weyl semimetals in terms of catalytic HER activity using EY as photosensitizer and triethanolamine as the sacrificial agent. It is hypothesized that the topology-related band inversion in MIrTe₄ Weyl semimetals promotes a high density of M d-states near the Fermi level, driving their high catalytic performance. This study introduces a new class of layered Weyl semimetals as efficient catalysts, and provides perspectives for designing topology-enhanced catalysts.

Can a generic magnetic insulator exhibit a Hall current? The quantum anomalous Hall effect (QAHE) is one example of an insulating bulk carrying a quantized Hall conductivity while insulators with zero Chern number present zero Hall conductance in the linear response regime. Here, we find that a general magnetic insulator possesses a nonlinear Hall conductivity quadratic to the electric field if the system breaks inversion symmetry, which can be identified as a new type of multiferroic coupling. This conductivity originates from an induced orbital magnetization due to virtual interband transitions. We identify three contributions to the wavepacket motion, a velocity shift, a positional shift, and a Berry curvature renormalization. In contrast to the crystalline solid, we find that this nonlinear Hall conductivity vanishes for Landau levels of a 2D electron gas, indicating a fundamental difference between the QAHE and the integer quantum Hall effect.

Nonlinear electrical response permits a unique window into effects of band structure geometry. It can be calculated either starting from a Boltzmann approach for small frequencies, or using Kubo's formula for resonances at finite frequency. However, a precise connection between both approaches has not been established. Focusing on the second order nonlinear response, here we show how the semiclassical limit can be recovered from perturbation theory in the velocity gauge, provided that finite quasiparticle lifetimes are taken into account. We find that matrix elements related to the band geometry combine in this limit to produce the semiclassical nonlinear conductivity. We demonstrate the power of the new formalism by deriving a quantum contribution to the nonlinear conductivity which is of order τ⁻¹ in the relaxation time τ, which is principally inaccessible within the Boltzmann approach. We outline which steps can be generalized to higher orders in the applied perturbation, and comment about potential experimental signatures of our results.

During the past two decades, it has been established that a non-trivial electron wave-function topology generates an anomalous Hall effect (AHE), which shows itself as a Hall conductivity non-linear in magnetic field. Here, we report on an unprecedented case of field-linear AHE. In Mn₃Sn, a kagome magnet, the out-of-plane Hall response, which shows an abrupt jump, was discovered to be a case of AHE. We find now that the in-plane Hall response, which is perfectly linear in magnetic field, is set by the Berry curvature of the wavefunction. The amplitude of the Hall response and its concomitant Nernst signal exceed by far what is expected in the semiclassical picture. We argue that magnetic field induces out-of-plane spin canting and thereafter gives rise to nontrivial spin chirality on the kagome lattice. In band structure, we find that the spin chirality modifies the topology by gapping out Weyl nodal lines unknown before, accounting for the AHE observed. Our work reveals intriguing unification of real-space Berry phase from spin chirality and momentum-space Berry curvature in a kagome material.

Dirac semimetals feature Dirac cones with topologically nontrivial states in the bulk that are protected by crystalline symmetries. They attract considerable attention due to rich quantum states and properties of interest, such as high Fermi velocities, mobility, and small effective masses. Here, we show that a ternary intermetallic BaAuSb crystal hosts both trivial and nontrivial topological Dirac states in the bulk. The nontrivial Fermi-surface pocket at the Brillouin zone center is characterized with only a few hundredths of a bare electron mass and with very high mobility. All parts of the Fermi surface detected by quantum oscillations, topologically trivial or nontrivial, have carriers with unusually high Fermi velocities and small masses. These conducting states may be coupled with magnetic moments in materials where Ba is replaced by magnetic rare-earth atoms.

The kagome lattice provides a fascinating playground to study geometrical frustration, topology and strong correlations. The newly discovered kagome metals AV3Sb5 (where A can refer to K, Rb or Cs) exhibit phenomena including topological band structure, symmetry-breaking charge-density waves and superconductivity. Nevertheless, the nature of the symmetry breaking in the charge-density wave phase is not yet clear, despite the fact that it is crucial in order to understand whether the superconductivity is unconventional. In this work, we perform scanning birefringence microscopy on all three members of this family and find that six-fold rotation symmetry is broken at the onset of the charge-density wave transition in all these compounds. We show that the three nematic domains are oriented at 120° to each other and propose that staggered charge-density wave orders with a relative π phase shift between layers is a possibility that can explain these observations. We also perform magneto-optical Kerr effect and circular dichroism measurements. The onset of both signals is at the transition temperature, indicating broken time-reversal symmetry and the existence of the long-sought loop currents in that phase.

Tailoring magnetic orders in topological insulators is critical to the realization of topological quantum phenomena. An outstanding challenge is to find a material where atomic defects lead to tunable magnetic orders while maintaining a nontrivial topology. Here, by combining magnetization measurements, angle-resolved photoemission spectroscopy, and transmission electron microscopy, we reveal disorder-enabled, tunable magnetic ground states in MnBi6Te10. In the ferromagnetic phase, an energy gap of 15 meV is resolved at the Dirac point on the MnBi2Te4 termination. In contrast, antiferromagnetic MnBi6Te10 exhibits gapless topological surface states on all terminations. Transmission electron microscopy and magnetization measurements reveal substantial Mn vacancies and Mn migration in ferromagnetic MnBi6Te10. We provide a conceptual framework where a cooperative interplay of these defects drives a delicate change of overall magnetic ground state energies and leads to tunable magnetic topological orders. Our work provides a clear pathway for nanoscale defect-engineering toward the realization of topological quantum phases.

The vanadium-based kagome superconductor CsV₃Sb₅ has attracted tremendous attention due to its unexcepted anomalous Hall effect (AHE), charge density waves (CDWs), nematicity, and a pseudogap pair density wave (PDW) coexisting with unconventional strong-coupling superconductivity. The origins of CDWs, unconventional superconductivity, and their correlation with different electronic states in this kagome system are of great significance, but so far, are still under debate. Chemical doping in the kagome layer provides one of the most direct ways to reveal the intrinsic physics, but remains unexplored. Here, we report, for the first time, the synthesis of Ti-substituted CsV₃Sb₅ single crystals and its rich phase diagram mapping the evolution of intertwining electronic states. The Ti atoms directly substitute for V in the kagome layers. CsV_3−xTi_xSb₅ shows two distinct superconductivity phases upon substitution. The Ti slightly-substituted phase displays an unconventional V-shaped superconductivity gap, coexisting with weakening CDW, PDW, AHE, and nematicity. The Ti highly-substituted phase has a U-shaped superconductivity gap concomitant with a short-range rotation symmetry breaking CDW, while long-range CDW, twofold symmetry of in-plane resistivity, AHE, and PDW are absent. Furthermore, we also demonstrate the chemical substitution of V atoms with other elements such as Cr and Nb, showing a different modulation on the superconductivity phases and CDWs. These findings open up a way to synthesise a new family of doped CsV₃Sb₅ materials, and further represent a new platform for tuning the different correlated electronic states and superconducting pairing in kagome superconductors.

We propose a novel heterostructure to achieve chiral topological superconductivity in two dimensions. A substrate with a large Rashba spin-orbit coupling energy is brought in proximity to a twisted bilayer of thin films exfoliated from a high-temperature cuprate superconductor. The combined system is then exposed to an out-of-plane magnetic field. The rare d + id pairing symmetry expected to occur in such a system allows for nontrivial topology; specifically, in contrast to the case of the twisted bilayer in isolation, the substrate induces an odd Chern number. The resulting phase is characterized by the presence of a Majorana zero mode in each vortex.

Magnetic topological insulators (MnBi₂Te₄)(Bi₂Te₃)_n were anticipated to exhibit magnetic energy gaps, while recent spectroscopic studies did not observe them. Thus, magnetism on the surface is under debate. In this work, we propose another symmetry criterion to probe surface magnetism. Because of both time-reversal symmetry breaking and inversion symmetry breaking, we demonstrate that the surface band structure violates momentum-inversion symmetry and leads to a threefold rather than sixfold rotational symmetry on the Fermi surface if corresponding surface states couple strongly to the surface magnetism. Such a momentum-inversion symmetry violation is significant along the Γ-K direction for surface bands on the (0001) plane, which serves as a criterion for determining the surface magnetism.

The electronic instabilities in CsV₃Sb₅ are believed to originate from the V 3d-electrons on the kagome plane, however the role of Sb 5p-electrons for 3-dimensional orders is largely unexplored. Here, using resonant tender X-ray scattering and high-pressure X-ray scattering, we report a rare realization of conjoined charge density waves (CDWs) in CsV₃Sb₅, where a 2 × 2 × 1 CDW in the kagome sublattice and a Sb 5p-electron assisted 2 × 2 × 2 CDW coexist. At ambient pressure, we discover a resonant enhancement on Sb L₁-edge (2s→5p) at the 2 × 2 × 2 CDW wavevectors. The resonance, however, is absent at the 2 × 2 × 1 CDW wavevectors. Applying hydrostatic pressure, CDW transition temperatures are separated, where the 2 × 2 × 2 CDW emerges 4 K above the 2 × 2 × 1 CDW at 1 GPa. These observations demonstrate that symmetry-breaking phases in CsV₃Sb₅ go beyond the minimal framework of kagome electronic bands near van Hove filling.

Boundary obstructed topological phases caused by Wannier orbital shift between ordinary atomic sites are proposed, which, however, cannot be indicated by symmetry eigenvalues at high symmetry momenta (symmetry indicators) in bulk. On the open boundary, Wannier charge centers can shift to different atoms from those in bulk, leading to in-gap surface states, higher-order hinge states or corner states. To demonstrate such orbital shift-induced boundary obstructed topological insulators, eight material candidates are predicted, all of which are overlooked in the present topological databases. Metallic surface states, hinge states, or corner states cover the large bulk energy gap (e.g., more than 1 eV in TlGaTe2) at related boundary, which are ready for experimental detection. Additionally, these materials are also fragile topological insulators with hourglass-like surface states.

Charge carriers in magic-angle graphene come in eight flavours described by a combination of their spin, valley and sublattice polarizations. When inversion and time-reversal symmetries are broken, this \u2018flavour\u2019 degeneracy can be lifted, and their corresponding bands can be sequentially filled. Due to their non-trivial band topology and Berry curvature, each band is classified by a topological Chern number C, leading to quantum anomalous Hall and Chern insulator states. Using a scanning superconducting quantum interference device on a tip, we image the nanoscale equilibrium orbital magnetism induced by the Berry curvature, the polarity of which is governed by C, and detect its two constituent components associated with the drift and self-rotation of the electronic wavepackets. At integer filling v\u2009=\u20091, we observe a zero-field Chern insulator, which\u2014rather than being described by a global topologically invariant C\u2014forms a mosaic of microscopic patches of C\u2009=\u2009−1, 0 or 1. On further filling, we find a first-order phase transition due to the recondensation of electrons from valley K to K\u2032, leading to irreversible flips of the local Chern number and magnetization, as well as to the formation of valley domain walls, giving rise to hysteretic anomalous Hall resistance.

Vortices are the hallmarks of hydrodynamic flow. Strongly interacting electrons in ultrapure conductors can display signatures of hydrodynamic behaviour, including negative non-local resistance1,2,3,4, higher-than-ballistic conduction5,6,7, Poiseuille flow in narrow channels8,9,10 and violation of the Wiedemann\u2013Franz law11. Here we provide a visualization of whirlpools in an electron fluid. By using a nanoscale scanning superconducting quantum interference device on a tip12, we image the current distribution in a circular chamber connected through a small aperture to a current-carrying strip in the high-purity type II Weyl semimetal WTe2. In this geometry, the Gurzhi momentum diffusion length and the size of the aperture determine the vortex stability phase diagram. We find that vortices are present for only small apertures, whereas the flow is laminar (non-vortical) for larger apertures. Near the vortical-to-laminar transition, we observe the single vortex in the chamber splitting into two vortices; this behaviour is expected only in the hydrodynamic regime and is not anticipated for ballistic transport. These findings suggest a new mechanism of hydrodynamic flow in thin pure crystals such that the spatial diffusion of electron momenta is enabled by small-angle scattering at the surfaces instead of the routinely invoked electron\u2013electron scattering, which becomes extremely weak at low temperatures. This surface-induced para-hydrodynamics, which mimics many aspects of conventional hydrodynamics including vortices, opens new possibilities for exploring and using electron fluidics in high-mobility electron systems.

Intense light\u2013matter interactions have revolutionized our ability to probe and manipulate quantum systems at sub-femtosecond timescales¹, opening routes to the all-optical control of electronic currents in solids at petahertz rates^2\u20137. Such control typically requires electric-field amplitudes in the range of almost volts per angstrom, when the voltage drop across a lattice site becomes comparable to the characteristic bandgap energies. In this regime, intense light\u2013matter interaction induces notable modifications to the electronic and optical properties^8\u201310, dramatically modifying the crystal band structure. Yet, identifying and characterizing such modifications remain an outstanding problem. As the oscillating electric field changes within the driving field\u2019s cycle, does the band structure follow and how can it be defined? Here we address this fundamental question, proposing all-optical spectroscopy to probe the laser-induced closing of the bandgap between adjacent conduction bands. Our work reveals the link between nonlinear light\u2013matter interactions in strongly driven crystals and the sub-cycle modifications in their effective band structure.

We employ polarization-resolved electronic Raman spectroscopy and density functional theory to study the primary and secondary order parameters, as well as their interplay, in the charge density wave (CDW) state of the kagome metal AV3Sb5. Previous x-ray diffraction data at 15 K established that the CDW order in CsV3Sb5 comprises of a 2×2×4 structure: one layer of inverse-star-of-David and three consecutive layers of star-of-David pattern. We analyze the lattice distortions based on the 2×2×4 structure at 15 K, and find that the U1 lattice distortion is the primarylike (leading) order parameter while M+1 and L−2 distortions are secondarylike order parameters for vanadium displacements. This conclusion is confirmed by the calculation of bare susceptibility χ\u20320(q) that shows a broad peak at around qz=0.25 along the hexagonal Brillouin zone face central line (U line). We also identify several phonon modes emerging in the CDW state, which are lattice vibration modes related to V and Sb atoms as well as alkali-metal atoms. The detailed temperature evolution of these modes' frequencies, half-width at half-maximums, and integrated intensities support a phase diagram with two successive structural phase transitions in CsV3Sb5: the first one with a primarylike order parameter appearing at TS=94K and the second isostructural one appearing at around T∗=70K. Furthermore, the T dependence of the integrated intensity for these modes shows two types of behavior below TS: the low-energy modes show a plateaulike behavior below T∗ while the high-energy modes monotonically increase below TS. These two behaviors are captured by the Landau free-energy model incorporating the interplay between the primarylike and the secondarylike order parameters via trilinear coupling. Especially, the sign of the trilinear term that couples order parameters with different wave vectors determines whether the primarylike and secondarylike order parameters cooperate or compete with each other, thus determining the shape of the T dependence of the intensities of Bragg peak in x-ray data and the amplitude modes in Raman data below TS. These results provide an accurate basis for studying the interplay between multiple CDW order parameters in kagome metal systems.

The bulk photovoltaic effect (BPVE) converts light into a coherent dc current at zero bias, through what is commonly known as the shift current. This current has previously been attributed to the displacement of the electronic wave function center in real space, when the sample is excited by light. We reveal that materials like twisted bilayer graphene (TBG) with a flatband dispersion are uniquely suited to maximize the BPVE because they lead to an enhanced shift in the momentum space, unlike any previously known shift current mechanism. We identify properties of quantum geometry, which go beyond the quantum geometric tensor, and are unrelated to Berry charges, as the physical origin of the large BPVE we observe in TBG. Our calculations show that TBG with a band gap of several meV exhibits a giant BPVE in a range of 0.2-1 THz, which represents the strongest BPVE reported so far at this frequency in a two-dimensional material and partially persists even a room temperature. Our paper provides a design principle for shift current generation, which applies to a broad range of twisted heterostructures with the potential to overcome the so-called "terahertz gap"in THz sensing.

Topological aspects of the geometry of DNA and similar chiral molecules have received a lot of attention, but the topology of their electronic structure is less explored. Previous experiments revealed that DNA can efficiently filter spin-polarized electrons between metal contacts, a process called chiral-induced spin selectivity. However, the underlying correlation between chiral structure and electronic spin remains elusive. In this work, we reveal an orbital texture in the band structure, a topological characteristic induced by the chirality. We found that this orbital texture enables the chiral molecule to polarize the quantum orbital. This orbital polarization effect (OPE) induces spin polarization assisted by the spin\u2013orbit interaction of a metal contact and leads to magnetoresistance and chiral separation. The orbital angular momentum of photoelectrons also plays an essential role in related photoemission experiments. Beyond chiral-induced spin selectivity, we predict that the orbital polarization effect could induce spin-selective phenomena even in achiral but inversion-breaking materials.

Twisted bilayer graphene (TBG) exhibits fascinating correlation-driven phenomena like the superconductivity and Mott insulating state, with flat bands and a chiral lattice structure. We find by quantum-transport calculations that the chirality leads to a giant unidirectional magnetoresistance (UMR) in TBG, where the unidirectionality refers to the resistance change under the reversal of the direction of current or magnetic field. We point out that flat bands significantly enhance this effect. The UMR increases quickly upon reducing the twist angle, and reaches about 20% for an angle of 1.5° in a 10 T in-plane magnetic field. We propose the band structure topology (asymmetry), which leads to a direction-sensitive mean free path, as a useful way to anticipate the UMR effect. The UMR provides a probe for chirality and band flatness in the twisted bilayers.

We carried out a comprehensive study of electronic transport, thermal, and thermodynamic properties in FeCr2Te4 single crystals. It exhibits bad-metallic behavior and anomalous Hall effect (AHE) below a weak-itinerant paramagnetic-to-ferrimagnetic transition Tc∼123 K. The linear scaling between the anomalous Hall resistivity ρxy and the longitudinal resistivity ρxx implies that the AHE in FeCr2Te4 is most likely dominated by an extrinsic skew-scattering mechanism rather than an intrinsic KL or an extrinsic side-jump mechanism, which is supported by our Berry phase calculations.

Using high-harmonic generation spectroscopy, we reveal the underlying attosecond dynamics in multi-band solid-state systems. We identify the mapping of spectral caustics into the high-harmonic spectrum, and probe the structure of multiple unpopulated high conduction bands.

We exploit a high-performing resistive-type trace oxygen sensor based on 2D high-mobility semiconducting Bi2O2Se nanoplates. Scanning tunneling microscopy combined with first-principle calculations confirms an amorphous Se atomic layer formed on the surface of 2D Bi2O2Se exposed to oxygen, which contributes to larger specific surface area and abundant active adsorption sites. Such 2D Bi2O2Se oxygen sensors have remarkable oxygen-adsorption induced variations of carrier density/mobility, and exhibit an ultrahigh sensitivity featuring minimum detection limit of 0.25 ppm, long-term stability, high durativity, and wide-range response to concentration up to 400 ppm at room temperature. 2D Bi2O2Se arrayed sensors integrated in parallel form are found to possess an oxygen detection minimum of sub-0.25 ppm ascribed to an enhanced signal-to-noise ratio. These advanced sensor characteristics involving ease integration show 2D Bi2O2Se is an ideal candidate for trace oxygen detection.

Silicon-based transistors are approaching their physical limits and thus new high-mobility semiconductors are sought to replace silicon in the microelectronics industry. Both bulk materials (such as silicon-germanium and III-V semiconductors) and low-dimensional nanomaterials (such as one-dimensional carbon nanotubes and two-dimensional transition metal dichalcogenides) have been explored, but, unlike silicon, which uses silicon dioxide (SiO2) as its gate dielectric, these materials suffer from the absence of a high-quality native oxide as a dielectric counterpart. This can lead to compatibility problems in practical devices. Here, we show that an atomically thin gate dielectric of bismuth selenite (Bi2SeO5) can be conformally formed via layer-by-layer oxidization of an underlying high-mobility two-dimensional semiconductor, Bi2O2Se. Using this native oxide dielectric, high-performance Bi2O2Se field-effect transistors can be created, as well as inverter circuits that exhibit a large voltage gain (as high as 150). The high dielectric constant (similar to 21) of Bi2SeO5 allows its equivalent oxide thickness to be reduced to 0.9 nm while maintaining a gate leakage lower than thermal SiO2. The Bi2SeO5 can also be selectively etched away by a wet chemical method that leaves the mobility of the underlying Bi2O2Se semiconductor almost unchanged.

Weyl semimetals exhibit unusual surface states and anomalous transport phenomena. It is hard to manipulate the band structure topology of specific Weyl materials. Topological transport phenomena usually appear at very low temperatures, which sets challenges for applications. In this work, we demonstrate the band topology modification via a weak magnetic field in a ferromagnetic Weyl semimetal candidate, Co2MnAl, at room temperature. We observe a tunable, giant anomalous Hall effect (AHE) induced by the transition involving Weyl points and nodal rings. The AHE conductivity is as large as that of a 3D quantum AHE, with the Hall angle (Theta (H)) reaching a record value (tan Theta H=0.21) at the room temperature among magnetic conductors. Furthermore, we propose a material recipe to generate large AHE by gaping nodal rings without requiring Weyl points. Our work reveals an intrinsically magnetic platform to explore the interplay between magnetic dynamics and topological physics for developing spintronic devices.

Nonlinear optical response is well studied in the context of semiconductors and has gained a renaissance in studies of topological materials in the recent decade. So far it mainly deals with nonmagnetic materials and it is believed to root in the Berry curvature of the material band structure. In this work we revisit the general formalism for the second-order optical response and focus on the consequences of the time-reversal-symmetry (T) breaking, by a diagrammatic approach. We have identified three physical mechanisms to generate a DC photocurrent, i.e., the Berry curvature, a term closely related to the quantum metric, and the diabatic motion. All three effects can be understood intuitively from the anomalous acceleration. The first two terms are respectively the antisymmetric and symmetric parts of the quantum geometric tensor. The last term is due to the dynamical antilocalization that appears from the phase accumulation between time-reversed fermion loops. Additionally, we derive the semiclassical conductivity that includes both intra- and interband effects. We find that T breaking can lead to a greatly enhanced nonlinear anomalous Hall effect that is beyond the contribution by the Berry curvature dipole.

Dual topological materials are unique topological phases that host coexisting surface states of different topological nature on the same or on different material facets. Here, we show that Bi
₂TeI is a dual topological insulator. It exhibits band inversions at two time reversal symmetry points of the bulk band, which classify it as a weak topological insulator with metallic states on its \u2018side\u2019 surfaces. The mirror symmetry of the crystal structure concurrently classifies it as a topological crystalline insulator. We investigated Bi
₂TeI spectroscopically to show the existence of both two-dimensional Dirac surface states, which are susceptible to mirror symmetry breaking, and one-dimensional channels that reside along the step edges. Their mutual coexistence on the step edge, where both facets join, is facilitated by momentum and energy segregation. Our observation of a dual topological insulator should stimulate investigations of other dual topology classes with distinct surface manifestations coexisting at their boundaries.

We demonstrate an anomalous spin-orbit torque induced by the broken magnetic symmetry in the antiferromagnet IrMn. We study the magnetic structure of three phases of IrMn thin films using neutron diffraction technique. The magnetic mirror symmetry M\u2032 is broken laterally in both L10-IrMn and L12-IrMn3 but not γ-IrMn3. We observe an out-of-plane dampinglike spin-orbit torque in both L10-IrMn/permalloy and L12-IrMn3/permalloy bilayers but not in γ-IrMn3/permalloy. This is consistent with both the symmetry analysis on the effects of a broken M\u2032 on spin-orbit torque and the theoretical predictions of the spin Hall effect and the Rashba-Edelstein effect. In addition, the measured spin-orbit torque efficiencies are 0.61 ± 0.01, 1.01 ± 0.03, and 0.80 ± 0.01 for the L10,L12, and γphases, respectively. Our work highlights the critical roles of the magnetic asymmetry in spin-orbit torque generation.

The Wiedemann-Franz (WF) law has been tested in numerous solids, but the extent of its relevance to the anomalous transverse transport and the topological nature of the wave function, remains an open question. Here, we present a study of anomalous transverse response in the noncollinear antiferromagnet Mn3Ge extended from room temperature down to sub-kelvin temperature and find that the anomalous Lorenz ratio remains close to the Sommerfeld value up to 100 K but not above. The finite-temperature violation of the WF correlation is caused by a mismatch between the thermal and electrical summations of the Berry curvature and not by inelastic scattering. This interpretation is backed by our theoretical calculations, which reveals a competition between the temperature and the Berry curvature distribution. The data accuracy is supported by verifying the anomalous Bridgman relation. The anomalous Lorenz ratio is thus an extremely sensitive probe of the Berry spectrum of a solid.

The search for unconventional superconductivity in Weyl semimetal materials is currently an exciting pursuit, since such superconducting phases could potentially be topologically non-trivial and host exotic Majorana modes. The layered material TaIrTe4 is a newly predicted time-reversal invariant type II Weyl semimetal with the minimum number of Weyl points. Here, we report the discovery of surface superconductivity in Weyl semimetal TaIrTe4. Our scanning tunneling microscopy/spectroscopy (STM/STS) visualizes Fermi arc surface states of TaIrTe4 that are consistent with the previous angle-resolved photoemission spectroscopy results. By a systematic study based on STS at ultralow temperature, we observe uniform superconducting gaps on the sample surface. The superconductivity is further confirmed by electrical transport measurements at ultralow temperature, with an onset transition temperature (T-c) up to 1.54 K being observed. The normalized upper critical field h*(T/T-c) behavior and the stability of the superconductivity against the ferromagnet indicate that the discovered superconductivity is unconventional with the p-wave pairing. The systematic STS, and thickness- and angular-dependent transport measurements reveal that the detected superconductivity is quasi-1D and occurs in the surface states. The discovery of the surface superconductivity in TaIrTe4 provides a new novel platform to explore topological superconductivity and Majorana modes.

The discovery of topological Weyl semimetals has revealed opportunities to realize several extraordinary physical phenomena in condensed matter physics. Specifically, Weyl semimetals with strong spin-orbit coupling, broken inversion symmetry, and novel spin textures are predicted to exhibit a large spin Hall effect that can efficiently convert the charge current to a spin current. Here, we report a direct experimental observation of large spin Hall and inverse spin Hall effects in the Weyl semimetal WTe2 at room temperature obeying the Onsager reciprocity relation. We demonstrate the detection of a pure spin current generated by the spin Hall phenomenon in WTe2 by making a van der Waals heterostructure with graphene, taking advantage of its long spin coherence length and spin transmission at the heterostructure interface. These experimental findings, well supported by ab initio calculations, show a large charge-spin conversion efficiency in WTe2, which can pave the way for the utilization of spin-orbit-induced phenomena in spintronic memory and logic circuit architectures.

The growing diversity of topological classes leads to ambiguity between classes that share similar boundary phenomenology. This is the status of bulk bismuth. Recent studies have classified it as either a strong or a higher-order topological insulator, both of which host helical modes on their boundaries. We resolve the topological classification of bismuth by spectroscopically mapping the response of its boundary modes to a screw-dislocation. We find that the one-dimensional mode, on step-edges, extends over a wide energy range and does not open a gap near the screw-dislocations. This signifies that this mode binds to the screw-dislocation, as expected for a material with nonzero weak indices. We argue that the small energy gap, at the time reversal invariant momentum L, positions bismuth within the critical region of a topological phase transition between a higher-order topological insulator and a strong topological insulator with nonzero weak indices.

Bulk-surface correspondence in Weyl semimetals ensures the formation of topological " Fermi arc" surface bands whose existence is guaranteed by bulk Weyl nodes. By investigating three distinct surface terminations of the ferromagnetic semimetal Co3Sn2S2, we verify spectroscopically its classification as a time-reversal symmetry-broken Weyl semimetal. We show that the distinct surface potentials imposed by three different terminations modify the Fermi-arc contour and Weyl node connectivity. On the tin (Sn) surface, we identify intra-Brillouin zone Weyl node connectivity of Fermi arcs, whereas on cobalt (Co) termination, the connectivity is across adjacent Brillouin zones. On the sulfur (S) surface, Fermi arcs overlap with nontopological bulk and surface states. We thus resolve both topologically protected and nonprotected electronic properties of a Weyl semimetal.

Surface Fermi arcs (SFAs), the unique open Fermi-surfaces (FSs) discovered recently in topological Weyl semimetals (TWSs), are unlike closed FSs in conventional materials and can give rise to many exotic phenomena, such as anomalous SFA-mediated quantum oscillations, chiral magnetic effects, three-dimensional quantum Hall effect, non-local voltage generation and anomalous electromagnetic wave transmission. Here, by using in-situ surface decoration, we demonstrate successful manipulation of the shape, size and even the connections of SFAs in a model TWS, NbAs, and observe their evolution that leads to an unusual topological Lifshitz transition not caused by the change of the carrier concentration. The phase transition teleports the SFAs between different parts of the surface Brillouin zone. Despite the dramatic surface evolution, the existence of SFAs is robust and each SFA remains tied to a pair of Weyl points of opposite chirality, as dictated by the bulk topology.

Spin-orbit torque (SOT) offers promising approaches to developing energy-efficient memory devices by electric switching of magnetization. Compared to other SOT materials, metallic antiferromagnet (AFM) potentially allows the control of SOT through its magnetic structure. Here, combining the results from neutron diffraction and spin-torque ferromagnetic resonance experiments, we show that the magnetic structure of epitaxially grown L1(0)-IrMn (a collinear AFM) is distinct from the widely presumed bulk one. It consists of twin domains, with the spin axes orienting toward [111] and [-111], respectively. This unconventional magnetic structure is responsible for much larger SOT efficiencies up to 0.60 +/- 0.04, compared to 0.083 +/- 0.002 for the polycrystalline IrMn. Furthermore, we reveal that this magnetic structure induces a large isotropic bulk contribution and a comparable anisotropic interfacial contribution to the SOT efficiency. Our findings shed light on the critical roles of bulk and interfacial antiferromagnetism to SOT generated by metallic AFM.

The spin Hall effect (SHE) is the conversion of charge current to spin current, and nonmagnetic metals with large SHEs are extremely sought after for spintronic applications, but their rarity has stifled widespread use. Here, we predict and explain the large intrinsic SHE in β-W and the A15 family of superconductors: W3Ta, Ta3Sb, and Cr3Ir having spin Hall conductivities (SHCs) of -2250, -1400, and 1210 (S/cm), respectively. Combining concepts from topological physics with the dependence of the SHE on the spin Berry curvature (SBC) of the electronic bands, we propose a simple strategy to rapidly search for materials with large intrinsic SHEs based on the following ideas: High symmetry combined with heavy atoms gives rise to multiple Dirac-like crossings in the electronic structure; without sufficient symmetry protection, these crossings gap due to spin-orbit coupling; and gapped crossings create large SBC.

We studied the nonlinear electric response in WTe₂ and MoTe₂ monolayers. When the inversion symmetry is breaking but the the time-reversal symmetry is preserved, a second-order Hall effect called the nonlinear anomalous Hall effect (NLAHE) emerges owing to the nonzero Berry curvature on the nonequilibrium Fermi surface. We reveal a strong NLAHE with a Hall-voltage that is quadratic with respect to the longitudinal current. The optimal current direction is normal to the mirror plane in these two-dimensional (2D) materials. The NLAHE can be sensitively tuned by an out-of-plane electric field, which induces a transition from a topological insulator to a normal insulator. Crossing the critical transition point, the magnitude of the NLAHE increases, and its sign is reversed. Our work paves the way to discover exotic nonlinear phenomena in inversion-symmetry-breaking 2D materials.

Spin-resolved band structures of L-gap surface states on Ag(111) and Cu(111) are investigated by spin- and angle-resolved photoelectron spectroscopy (SARPES) with a vacuum-ultraviolet laser. The observed spin textures of the Ag(111) and Cu(111) surface states agree with that expected by the conventional Rashba effect. The Rashba parameter of the Ag(111) surface state is estimated quantitatively and is 80% of that of Cu(111). The surface-state wave function is found to be predominantly of even mirror symmetry with negligible odd contribution by SARPES using a linearly polarized light. The results are consistent with our theoretical calculations for the orbital-resolved surface state.

Recent years have seen the rising importance of interface stacking in determining the electronic properties of multilayer materials stemming from the interlayer coupling; however, the stacking effects on exotic topological quantum orders largely remain to be explored. Here, we show by first-principles studies that bilayer Bi2Te3 host stacking is dependent on quantum spin Hall effects, with a topological phase transition induced by a change in the interlayer stacking pattern. The spin-filtered helical edge states are concomitantly switched on/off along with the changing interlayer stacking pattern. Since few-layer Bi2Te3 has already been experimentally synthesized, the present finding opens an avenue for exploring the fundamental mechanisms and the practical implications of the quantum phenomena associated with band topology in this versatile and intriguing 2D material. Published by AIP Publishing.

Exotic electronic states are realized in novel quantum materials. This field is revolutionized by the topological classification of materials. Such compounds necessarily host unique states on their boundaries. Scanning tunneling microscopy studies of these surface states have provided a wealth of spectroscopic characterization, with the successful cooperation of ab initio calculations. The method of quasiparticle interference imaging proves to be particularly useful for probing the dispersion relation of the surface bands. Herein, how a variety of additional fundamental electronic properties can be probed via this method is reviewed. It is demonstrated how quasiparticle interference measurements entail mesoscopic size quantization and the electronic phase coherence in semiconducting nanowires; helical spin protection and energy-momentum fluctuations in a topological insulator; and the structure of the Bloch wave function and the relative insusceptibility of topological electronic states to surface potential in a topological Weyl semimetal.

Three-dimensional topological semi-metals carry quasiparticle states that mimic massless relativistic Dirac fermions, elusive particles that have never been observed in nature. As they appear in the solid body, they are not bound to the usual symmetries of space-time and thus new types of fermionic excitations that explicitly violate Lorentz-invariance have been proposed, the so-called type-II Dirac fermions. We investigate the electronic spectrum of the transition-metal dichalcogenide PtSe2 by means of quantum oscillation measurements in fields up to 65 T. The observed Fermi surfaces agree well with the expectations from band structure calculations, that recently predicted a type-II Dirac node to occur in this material. A hole- and an electron-like Fermi surface dominate the semi-metal at the Fermi level. The quasiparticle mass is significantly enhanced over the bare band mass value, likely by phonon renormalization. Our work is consistent with the existence of type-II Dirac nodes in PtSe2, yet the Dirac node is too far below the Fermi level to support free Dirac-fermion excitations.

Recent interest in topological semimetals has led to the proposal ofmany newtopological phases that can be realized in real materials. Next to Dirac and Weyl systems, these include more exotic phases based on manifold band degeneracies in the bulk electronic structure. The exotic states in topological semimetals are usually protected by some sort of crystal symmetry, and the introduction of magnetic order can influence these states by breaking time-reversal symmetry. We show that we can realize a rich variety of different topological semimetal states in a single material, CeSbTe. This compound can exhibit different types ofmagnetic order that can be accessed easily by applying a small field. Therefore, it allows for tuning the electronic structure and can drive it through a manifold of topologically distinct phases, such as the first nonsymmorphic magnetic topological phase with an eightfold band crossing at a high-symmetry point. Our experimental results are backed by a full magnetic group theory analysis and ab initio calculations. This discovery introduces a realistic and promising platform for studying the interplay of magnetism and topology. We also show that we can generally expand the numbers of space groups that allow for high-order band degeneracies by introducing antiferromagnetic order.

Noncentrosymmetric metals are anticipated to exhibit a dc photocurrent in the nonlinear optical response caused by the Berry curvature dipole in momentum space. Weyl semimetals (WSMs) are expected to be excellent candidates for observing these nonlinear effects because they carry a large Berry curvature concentrated in small regions, i.e., near the Weyl points. We have implemented the semiclassical Berry curvature dipole formalism into an ab initio scheme and investigated the second-order nonlinear response for two representative groups of materials: the TaAs-family type-I WSMs and the MoTe2-family type-II WSMs. Both types of WSMs exhibited a Berry curvature dipole in which type-II Weyl points are usually superior to the type-I WSM because of the strong tilt. Corresponding nonlinear susceptibilities in several materials promise a nonlinear Hall effect in the dc field limit, which is within the experimentally detectable range.

Noncollinear antiferromagnets, such as Mn-3 Sn and Mn-3 Ir, were recently shown to be analogous to ferromagnets in that they have a large anomalous Hall effect. Here we show that these materials are similar to ferromagnets in another aspect: the charge current in these materials is spin polarized. In addition, we show that the same mechanism that leads to the spin-polarized current also leads to a transverse spin current, which has a distinct symmetry and origin from the conventional spin Hall effect. We illustrate the existence of the spin-polarized current and the transverse spin current by performing ab initio microscopic calculations and by analyzing the symmetry. We discuss possible applications of these novel spin currents, such as an antiferromagnetic metallic or tunneling junction.

Topological insulators represent unusual topological quantum states, typically with gapped bulk band structure but gapless surface Dirac fermions protected by time-reversal symmetry. Recently, a distinct kind of topological insulator resulting from nonsymmorphic crystalline symmetry was proposed in the KHgX (X=As, Sb, Bi) compounds. Unlike regular topological crystalline insulators, the nonsymmorphic glide-reflection symmetry in KHgX guarantees the appearance of an exotic surface fermion with hourglass shape dispersion (where two pairs of branches switch their partners) residing on its (010) side surface, contrasting to the usual two-dimensional Dirac fermion form. Here, by using high-resolution angle-resolved photoemission spectroscopy, we systematically investigate the electronic structures of KHgSb on both (001) and (010) surfaces and reveal the unique in-gap surface states on the (010) surface with delicate dispersion consistent with the "hourglass Fermion" recently proposed. Our experiment strongly supports that KHgSb is a nonsymmorphic topological crystalline insulator with hourglass fermions, which serves as an important step to the discovery of unique topological quantum materials and exotic fermions protected by nonsymmorphic crystalline symmetry.

The conservation laws, such as those of charge, energy and momentum, have a central role in physics. In some special cases, classical conservation laws are broken at the quantum level by quantum fluctuations, in which case the theory is said to have quantum anomalies. One of the most prominent examples is the chiral anomaly, which involves massless chiral fermions. These particles have their spin, or internal angular momentum, aligned either parallel or antiparallel with their linear momentum, labelled as left and right chirality, respectively. In three spatial dimensions, the chiral anomaly is the breakdown (as a result of externally applied parallel electric and magnetic fields) of the classical conservation law that dictates that the number of massless fermions of each chirality are separately conserved. The current that measures the difference between left- and right-handed particles is called the axial current and is not conserved at the quantum level. In addition, an underlying curved space-time provides a distinct contribution to a chiral imbalance, an effect known as the mixed axial-gravitational anomaly, but this anomaly has yet to be confirmed experimentally. However, the presence of a mixed gauge-gravitational anomaly has recently been tied to thermoelectrical transport in a magnetic field, even in flat space-time, suggesting that such types of mixed anomaly could be experimentally probed in condensed matter systems known as Weyl semimetals. Here, using a temperature gradient, we observe experimentally a positive magneto-thermoelectric conductance in the Weyl semimetal niobium phosphide (NbP) for collinear temperature gradients and magnetic fields that vanishes in the ultra-quantum limit, when only a single Landau level is occupied. This observation is consistent with the presence of a mixed axial-gravitational anomaly, providing clear evidence for a theoretical concept that has so far eluded experimental detection.

We have found Dirac nodal lines (DNLs) in the band structures of metallic rutile oxides IrO2, OsO2, and RuO2 and have revealed a large spin Hall conductivity contributed by these nodal lines, which explains a strong spin Hall effect (SHE) of IrO2 discovered recently. Two types of DNLs exist. The first type forms DNL networks that extend in the whole Brillouin zone and appears only in the absence of spin-orbit coupling (SOC), which induces surface states on the boundary. Because of SOC-induced band anticrossing, a large intrinsic SHE can be realized in these compounds. The second type appears at the Brillouin zone edges and is stable against SOC because of the protection of nonsymmorphic symmetry. Besides reporting these DNL materials, our work reveals the general relationship between DNLs and the SHE, indicating a way to apply Dirac nodal materials for spintronics.

We report superconductive iridium pnictides Ba_xIr₄X₁₂ (X = As and P) with a filled skutterudite structure, demonstrating that Ba filling dramatically alters their electronic properties and induces a nonmetal-to-metal transition with increasing the Ba content x. The highest superconducting transition temperatures are 4.8 and 5.6 K observed for Ba_xIr₄As₁₂ and Ba_xIr₄P₁₂, respectively. The superconductivity in Ba_xIr₄X₁₂ can be classified into the Bardeen-Cooper-Schrieffer type with intermediate coupling.

The search for highly efficient and low-cost catalysts is one of the main driving forces in catalytic chemistry. Current strategies for the catalyst design focus on increasing the number and activity of local catalytic sites, such as the edge sites of molybdenum disulfides in the hydrogen evolution reaction (HER). Here, the study proposes and demonstrates a different principle that goes beyond local site optimization by utilizing topological electronic states to spur catalytic activity. For HER, excellent catalysts have been found among the transition-metal monopnictides\u2014NbP, TaP, NbAs, and TaAs\u2014which are recently discovered to be topological Weyl semimetals. Here the study shows that the combination of robust topological surface states and large room temperature carrier mobility, both of which originate from bulk Dirac bands of the Weyl semimetal, is a recipe for high activity HER catalysts. This approach has the potential to go beyond graphene based composite photocatalysts where graphene simply provides a high mobility medium without any active catalytic sites that have been found in these topological materials. Thus, the work provides a guiding principle for the discovery of novel catalysts from the emerging field of topological materials.

A pressure-induced topological quantum phase transition has been theoretically predicted for the semiconductor bismuth tellurohalide BiTeI with giant Rashba spin splitting. In this work, evolution of the electrical transport properties in BiTeI and BiTeBr is investigated under high pressure. The pressure-dependent resistivity in a wide temperature range passes through a minimum at around 3 GPa, indicating the predicted topological quantum phase transition in BiTeI. Superconductivity is observed in both BiTeI and BiTeBr, while resistivity at higher temperatures still exhibits semiconducting behavior. Theoretical calculations suggest that superconductivity may develop from the multivalley semiconductor phase. The superconducting transition temperature, T_c, increases with applied pressure and reaches a maximum value of 5.2 K at 23.5 GPa for BiTeI (4.8 K at 31.7 GPa for BiTeBr), followed by a slow decrease. The results demonstrate that BiTeX (X = I, Br) compounds with nontrivial topology of electronic states display new ground states upon compression.

The class of topological semimetals comprises a large pool of compounds. Together they provide a wide platform to realize exotic quasiparticles, for example, Dirac, nodal-line Dirac, and Weyl fermions. In this Rapid Communication, we report the Berry phase, Fermi-surface topology, and anisotropic magnetoresistance of HfSiS which has recently been predicted to be a nodal-line semimetal. This compound contains a large carrier density, higher than most of the known semimetals. Massive amplitudes of de Haas-van Alphen and Shubnikov-de Haas oscillations up to 20 K in 7 T assist us in witnessing a nontrivial π-Berry phase, which is a consequence of topological Dirac-type dispersion of bands originating from the hybridization of px+py and dx2-y2 orbitals of square-net plane of Si and Hf atoms, respectively. Furthermore, we establish the three-dimensional Fermi surface which consists of very asymmetric water caltroplike electrons and barley seedlike hole pockets which account for the anisotropic magnetoresistance in HfSiS.

We have carried out a comprehensive study of the intrinsic anomalous Hall effect and spin Hall effect of several chiral antiferromagnetic compounds Mn3X (X = Ge, Sn, Ga, Ir, Rh and Pt) by ab initio band structure and Berry phase calculations. These studies reveal large and anisotropic values of both the intrinsic anomalous Hall effect and spin Hall effect. The Mn3X materials exhibit a noncollinear antiferromagnetic order which, to avoid geometrical frustration, forms planes of Mn moments that are arranged in a Kagome-type lattice. With respect to these Kagome planes, we find that both the anomalous Hall conductivity (AHC) and the spin Hall conductivity (SHC) are quite anisotropic for any of these materials. Based on our calculations, we propose how to maximize AHC and SHC for different materials. The band structures and corresponding electron filling, that we show are essential to determine the AHC and SHC, are compared for these different compounds. We point out that Mn3Ga shows a large SHC of about 600 (/e)(Ωcm)-1. Our work provides insights into the realization of strong anomalous Hall effects and spin Hall effects in chiral antiferromagnetic materials.

Topological Dirac semimetals (DSMs) exhibit nodal points through which energy bands disperse linearly in three-dimensional (3D) momentum space, a 3D analog of graphene. The first experimentally confirmed DSMs with a pair of Dirac points (DPs), Na3Bi and Cd3As2, show topological surface Fermi arc states and exotic magnetotransport properties, boosting the interest in the search for stable and nontoxic DSM materials. Based on density-functional theory and dynamical mean-field theory calculations, we predict a family of palladium and platinum oxides to be robust 3D DSMs with three pairs of Dirac points that are well separated from bulk bands. The Fermi arcs at the surface display a Lifshitz transition upon a continuous change of the chemical potential. Corresponding oxides are already available as high-quality single crystals, an excellent precondition for the verification of our predictions by photoemission and magnetotransport experiments, extending DSMs to the versatile family of transition-metal oxides.

The rare-earth monopnictide LaBi exhibits exotic magneto-transport properties, including an extremely large and anisotropic magnetoresistance. Experimental evidence for topological surface states is still missing although band inversions have been postulated to induce a topological phase in LaBi. In this work, we have revealed the existence of surface states of LaBi through the observation of three Dirac cones: two coexist at the corners and one appears at the centre of the Brillouin zone, by employing angle-resolved photoemission spectroscopy in conjunction with ab initio calculations. The odd number of surface Dirac cones is a direct consequence of the odd number of band inversions in the bulk band structure, thereby proving that LaBi is a topological, compensated semimetal, which is equivalent to a time-reversal invariant topological insulator. Our findings provide insight into the topological surface states of LaBi's semi-metallicity and related magneto-transport properties.

We investigated the electronic structure of the layered transition-metal dichalcogenides VS₂ and VSe₂ by first-principles calculations. Both compounds exhibit metal-insulator transitions when crossing over from the bulk to the two-dimensional monolayer. In the monolayer limit, the Coulomb interaction is enhanced due to the dimension reduction, leading to the insulating state. Moreover, these monolayers are found to be ferromagnetic, supplying excellent candidates for ferromagnetic insulators. When increasing the thickness, the few-layer structure turns metallic and presents large anomalous Hall conductivity (∼100 S/cm), which oscillates with respect to the thickness due to the size effect. Our findings presents profound materials, such as ferromagnetic insulators and anomalous Hall ferromagnets, for the spintronic application.

Tantalum arsenide is a member of the noncentrosymmetric monopnictides, which are putative Weyl semimetals. In these materials, three-dimensional chiral massless quasiparticles, the so-called Weyl fermions, are predicted to induce novel quantum mechanical phenomena, such as the chiral anomaly and topological surface states. However, their chirality is only well defined if the Fermi level is close enough to the Weyl points that separate Fermi surface pockets of opposite chirality exist. In this Letter, we present the bulk Fermi surface topology of high quality single crystals of TaAs, as determined by angle-dependent Shubnikov-de Haas and de Haas-van Alphen measurements combined with ab initio band-structure calculations. Quantum oscillations originating from three different types of Fermi surface pockets were found in magnetization, magnetic torque, and magnetoresistance measurements performed in magnetic fields up to 14 T and temperatures down to 1.8 K. Of these Fermi pockets, two are pairs of topologically nontrivial electron pockets around the Weyl points and one is a trivial hole pocket. Unlike the other members of the noncentrosymmetric monopnictides, TaAs is the first Weyl semimetal candidate with the Fermi energy sufficiently close to both types of Weyl points to generate chiral quasiparticles at the Fermi surface.

Wereport the existence of the quantum spin Hall effect (QSHE) in monolayers of transition-metal carbidesMC(M=Zr, Hf). Under ambient conditions, the ZrC monolayer exhibits QSHE with an energy gap of 54 meV, in which topological helical edge states exist. Enhanced d_xy-d_xy interaction induces band inversion, resulting in nontrivial topological features. By applying in-plane strain, the HfC monolayer can be tuned from a trivial insulator to a quantum spin Hall insulator with an energy gap of 170 meV, three times that of the ZrC monolayer. The strong stability of MC monolayers provides a new platform for QSHE and spintronic applications.

There has been considerable interest in spin-orbit torques for the purpose of manipulating the magnetization of ferromagnetic elements for spintronic technologies. Spin-orbit torques are derived from spin currents created from charge currents in materials with significant spin-orbit coupling that propagate into an adjacent ferromagnetic material. A key challenge is to identify materials that exhibit large spin Hall angles, that is, efficient charge-to-spin current conversion. Using spin torque ferromagnetic resonance, we report the observation of a giant spin Hall angle θ^eff_SH of up to ~0.35 in (001)-oriented single-crystalline antiferromagnetic IrMn₃ thin films, coupled to ferromagnetic permalloy layers, and a θ^eff_SH that is about three times smaller in (111)-oriented films. For (001)-oriented samples, we show that the magnitude of θ^eff_SH can be significantly changed by manipulating the populations of various antiferromagnetic domains through perpendicular field annealing. We identify two distinct mechanisms that contribute to θ^eff_SH: the first mechanism, which is facet-independent, arises from conventional bulk spin-dependent scattering within the IrMn₃ layer, and the second intrinsic mechanism is derived from the unconventional antiferromagnetic structure of IrMn₃. Using ab initio calculations, we show that the triangular magnetic structure of IrMn₃ gives rise to a substantial intrinsic spin Hall conductivity that is much larger for the (001) than for the (111) orientation, consistent with our experimental findings.

Topological quantum materials represent a new class of matter with both exotic physical phenomena and novel application potentials. Many Heusler compounds, which exhibit rich emergent properties such as unusual magnetism, superconductivity and heavy fermion behaviour, have been predicted to host non-trivial topological electronic structures. The coexistence of topological order and other unusual properties makes Heusler materials ideal platform to search for new topological quantum phases (such as quantum anomalous Hall insulator and topological superconductor). By carrying out angle-resolved photoemission spectroscopy and ab initio calculations on rare-earth half-Heusler compounds LnPtBi (Ln=Lu, Y), we directly observe the unusual topological surface states on these materials, establishing them as first members with non-trivial topological electronic structure in this class of materials. Moreover, as LnPtBi compounds are non-centrosymmetric superconductors, our discovery further highlights them as promising candidates of topological superconductors.

The discovery of superconductivity in hafnium pentatelluride HfTe5 under high pressure is reported. Two structural phase transitions and metallization with superconductivity developing at around 5 GPa are observed. A maximal critical temperature of 4.8 K is attained at a pressure of 20 GPa, and superconductivity persists up to the maximum pressure of the study (42 GPa). The combination of electrical transport and crystal structure measurements as well as theoretical electronic structure calculations enables the construction of a phase diagram of HfTe5 under high pressure.

Topological insulators are characterized by an inverted band structure in the bulk and metallic surface states on the surface. In LaBi, a semimetal with a band inversion equivalent to a topological insulator, we observe surface-state-like behavior in the magnetoresistance. The electrons responsible for this pseudo-two-dimensional transport, however, originate from the bulk states rather topological surface states, which is witnessed by the angle-dependent quantum oscillations of the magnetoresistance and ab initio calculations. As a consequence, the magnetoresistance exhibits strong anisotropy with large amplitude (∼105%).

Starting from the three-dimensional Dirac semimetal in Na3Bi, we found a topological insulator (TI) in the known compound of NaBaBi by extra pressure. The TI of NaBaBi can be viewed as the distorted version of Na3Bi with breaking inversion symmetry. When the exchange-correlation energy is considered in generalized gradient approximation (GGA), the TI phase has a band inversion between the Bi-p and Na-s orbitals. Since GGA often overestimates the band inversion, we also performed more accurate calculations by using hybrid functional theory (HSE). From HSE calculations we found that NaBaBi exhibits as a trivial insulator at zero pressure, and the other TI phase with p-d inversion can be achieved by pressure. Though both of two TI phases have Dirac-cone-type surface states, they have opposite spin textures. In the upper cone, a lefthanded spin texture exists for the s-p inverted phase (similar to a common TI, e.g., Bi2Se3), whereas a righthanded spin texture appears for the p-d inverted phase. This work presents a prototype model of a TI exhibits righthanded spin texture.

Using first-principles density-functional theory, we have investigated the electronic and magnetic properties of recently synthesized and characterized 5d double-perovskites Sr2BOsO6(B=Y,In,Sc). The electronic structure calculations show that in all compounds the Os5+ (5d3) site is the only magnetically active one, whereas Y3+, In3+, and Sc3+ remain in nonmagnetic states with Sc/Y and In featuring d0 and d10 electronic configurations, respectively. Our studies reveal the important role of closed-shell (d10) versus open-shell (d0) electronic configurations of the nonmagnetic sites in determining the overall magnetic exchange interactions. Although the magnetic Os5+ (5d3) site is the same in all compounds, the magnetic superexchange interactions mediated by nonmagnetic Y/In/Sc species are strongest for Sr2ScOsO6, weakest for Sr2InOsO6, and intermediate in the case of the Y (d0) due to different energy overlaps between Os-5d and Y/In/Sc-d states. This explains the experimentally observed substantial differences in the magnetic transition temperatures of these materials, despite an identical magnetic site and underlying magnetic ground state. Furthermore, short-range Os-Os exchange interactions are more prominent than long-range Os-Os interactions in these compounds, which contrasts with the behavior of other 3d-5d double perovskites.

The Weyl semimetal NbP was found to exhibit topological Fermi arcs and exotic magnetotransport properties. Here, we report on magnetic quantum-oscillation measurements on NbP and construct the three-dimensional Fermi surface with the help of band-structure calculations. We reveal a pair of spin-orbit-split electron pockets at the Fermi energy and a similar pair of hole pockets, all of which are strongly anisotropic. The Weyl points that are located in the kz≈π/c plane are found to exist 5 meV above the Fermi energy. Therefore, we predict that the chiral anomaly effect can be realized in NbP by electron doping to drive the Fermi energy to the Weyl points.

Topological Weyl semimetals (TWSs) represent a novel state of topological quantum matter which not only possesses Weyl fermions (massless chiral particles that can be viewed as magnetic monopoles in momentum space) in the bulk and unique Fermi arcs generated by topological surface states, but also exhibits appealing physical properties such as extremely large magnetoresistance and ultra-high carrier mobility. Here, by performing angle-resolved photoemission spectroscopy (ARPES) on NbP and TaP, we directly observed their band structures with characteristic Fermi arcs of TWSs. Furthermore, by systematically investigating NbP, TaP and TaAs from the same transition metal monopnictide family, we discovered their Fermiology evolution with spin-orbit coupling (SOC) strength. Our experimental findings not only reveal the mechanism to realize and fine-tune the electronic structures of TWSs, but also provide a rich material base for exploring many exotic physical phenomena (for example, chiral magnetic effects, negative magnetoresistance, and the quantum anomalous Hall effect) and novel future applications.

Exotic and robust metallic surface states of topological insulators (TIs) have been expected to provide a promising platform for novel surface chemistry and catalysis. However, it is still not fully known how TIs affect the activity of catalysts. In this work, we study the effects of topological surface states (TSSs) on the activity of transition metal clusters (Au, Ag, Cu, Pt, and Pd), which are supported on a TI Bi₂Se₃ substrate. It was found the adsorption energy of oxygen on the supported catalysts can be always enhanced due to the TSSs. However, it does not necessarily mean an increase of the activity in catalytic oxidation reaction. Rather, the enhanced adsorption behavior in the presence of TSSs exhibits dual effects, determined by the intrinsic reactivity of these catalysts with oxygen. For the Au case, the activity of catalytic oxidation can be improved because the TSSs can enhance the dissociation rate of dioxygen. In contrast, a negative effect is found for the Pt and Pd clusters since the TSSs will suppress the desorption process of reaction products. We also found that the effect of TSSs on the activity of hydrogen evolution reaction (HER) is quite similar (i.e., the metals with original weak reactivity can gain a positive effect from TSSs). The present work can pave a way for more rational design and selection of catalysts when using TIs as substrates.

We investigate the orthorhombic phase (Td) of the layered transition-metal dichalcogenide MoTe2 as a Weyl semimetal candidate. MoTe2 exhibits four pairs of Weyl points lying slightly above (∼6meV) the Fermi energy in the bulk band structure. Different from its cousin WTe2, which was recently predicted to be a type-II Weyl semimetal, the spacing between each pair of Weyl points is found to be as large as 4% of the reciprocal lattice in MoTe2 (six times larger than that of WTe2). When projected onto the surface, the Weyl points are connected by Fermi arcs, which can be easily accessed by angle-resolved photoemission spectroscopy due to the large Weyl point separation. In addition, we show that the correlation effect or strain can drive MoTe2 from a type-II to a type-I Weyl semimetal.

Very recently the topological Weyl semimetal (WSM) state was predicted in the noncentrosymmetric compounds NbP, NbAs, TaP, and TaAs and soon led to photoemission and transport experiments to verify the presumed topological properties such as Fermi arcs (unclosed Fermi surfaces) and the chiral anomaly. In this work we have performed fully ab initio calculations of the surface band structures of these four WSM materials and revealed the Fermi arcs with spin-momentum-locked spin texture. On the (001) polar surface, the shape of the Fermi surface depends sensitively on the surface terminations (cations or anions), although they exhibit the same topology with arcs. The anion (P or As) terminated surfaces are found to fit recent photoemission measurements well. Such surface potential dependence indicates that the shape of the Fermi surface can be sensitively manipulated by depositing guest species (such as K atoms), as we demonstrate. On the polar surface of a WSM without inversion symmetry, Rashba-type spin polarization naturally exists in the surface states and leads to strong spin texture. By tracing the spin polarization of the Fermi surface, one can distinguish Fermi arcs from trivial Fermi circles. The four compounds NbP, NbAs, TaP, and TaAs present an increasing amplitude of spin-orbit coupling (SOC) in band structures. By comparing their surface states, we reveal the evolution of topological Fermi arcs from the spin-degenerate Fermi circle to spin-split arcs when the SOC increases from zero to a finite value. Our work presents a comprehensive understanding of the topological surface states of WSMs, which will especially be helpful for future spin-revolved photoemission and transport experiments.

Recent experiments have revealed spectacular transport properties in semimetals, such as the large, non-saturating magnetoresistance exhibited by WTe 2 (ref.). Topological semimetals with massless relativistic electrons have also been predicted as three-dimensional analogues of graphene. These systems are known as Weyl semimetals, and are predicted to have a range of exotic transport properties and surface states, distinct from those of topological insulators. Here we examine the magneto-transport properties of NbP, a material the band structure of which has been predicted to combine the hallmarks of a Weyl semimetal with those of a normal semimetal. We observe an extremely large magnetoresistance of 850,000% at 1.85 K (250% at room temperature) in a magnetic field of up to 9 T, without any signs of saturation, and an ultrahigh carrier mobility of 5 × 10 6 cm 2 V â '1 s â '1 that accompanied by strong Shubnikov-de Haas (SdH) oscillations. NbP therefore presents a unique example of a material combining topological and conventional electronic phases, with intriguing physical properties resulting from their interplay.

Recent theoretical studies employing density-functional theory have predicted BaBiO₃ (when doped with electrons) and YBiO₃ to become a topological insulator (TI) with a large topological gap (∼0.7 eV). This, together with the natural stability against surface oxidation, makes the Bismuth-Oxide family of special interest for possible applications in quantum information and spintronics. The central question, we study here, is whether the hole-doped Bismuth Oxides, i.e. Ba_1-xK_xBiO₃ and BaPb_1-xBi_xO₃, which are "high-Tc" bulk superconducting near 30 K, additionally display in the further vicinity of their Fermi energy E_F a topological gap with a Dirac-type of topological surface state. Our electronic structure calculations predict the K-doped family to emerge as a TI, with a topological gap above E_F. Thus, these compounds can become superconductors with hole-doping and potential TIs with additional electron doping. Furthermore, we predict the Bismuth-Oxide family to contain an additional Dirac cone below E_F for further hole doping, which manifests these systems to be candidates for both electron- and hole-doped topological insulators.

Local environments and valence electron counts primarily determine the electronic states and physical properties of transition-metal complexes. For example, square-planar coordination geometries found in transition-metal oxometalates such as cuprates are usually associated with the d⁸ or d⁹ electron configuration. In this work, we address an unusual square-planar single oxoanionic [IrO₄]^4- species, as observed in Na₄IrO₄ in which Ir^IV has a d⁵ configuration, and characterize the chemical bonding through experiments and by ab initio calculations. We find that the Ir^IV center in ground-state Na₄IrO₄ has square-planar coordination geometry because of the weak Coulomb repulsion of the Ir-5d electrons. In contrast, in its 3d counterpart Na₄CoO₄, the Co^IV center is tetrahedrally coordinated because of strong electron correlation. Na₄IrO₄ may thus serve as a simple yet important example to study the ramifications of Hubbard-type Coulomb interactions on local geometries.

We have performed ab initio band-structure calculations on more than 2000 half-Heusler compounds in order to search for new candidates for topological insulators. Herein, LiAuS and NaAuS are found to be the strongest topological insulators with the bulk band gaps of 0.20 and 0.19 eV, respectively, different from the zero band-gap feature reported in other Heusler topological insulators. Due to the inversion asymmetry of the Heusler structure, their topological surface states on the top and bottom surfaces exhibit p-type and n-type carriers, respectively. Thus, these materials may serve as an ideal platform for the realization of topological magnetoelectric effects as polar topological insulators. Moreover, these topological surface states exhibit the right-hand spin texture in the upper Dirac cone, which distinguishes them from currently known topological insulator materials. Their topological nontrivial character remains robust against in-plane strains, which makes them suitable for epitaxial growth of films.

Double perovskites Sr₂BOsO₆ (B = Y, In, and Sc) were prepared from the respective binary metal oxides, and their structural, magnetic, and electronic properties were investigated. At room temperature all these compounds crystallize in the monoclinic space group P2₁/n. They contain magnetic osmium (Os⁵⁺, t_2g³) ions and are antiferromagnetic insulators with Néel temperatures TN = 53 K, 26 K, and 92 K for B = Y, In, and Sc, respectively. Powder neutron diffraction studies on Sr₂YOsO₆ and Sr₂InOsO₆ showed that the crystal structures remain unchanged down to 3 K. The Y and In compounds feature a type I antiferromagnetic spin structure with ordered Os moments of 1.91 μ_B and 1.77 μ_B, respectively. The trend in TN does not simply follow the development of the lattice parameters, which suggests that d⁰ compared to d¹⁰ ions on the B site favor a somewhat different balance of exchange interactions in the frustrated Os⁵⁺ fcc-like lattice.

Topological insulators are known for their metallic surface states, a result of strong spin-orbit coupling, that exhibit unique surface transport phenomenon. However, these surface transport phenomena are buried in the presence of metallic bulk conduction. We synthesized very high quality Bi2Te2Se single crystals by using a modified Bridgman method that possess high bulk resistivity of >20 Ωcm below 20 K, whereas the bulk is mostly inactive and surface transport dominates. The temperature dependence of resistivity follows an activation law like a gap semiconductor in temperature range 20-300 K. To extract the surface transport from that of the bulk, we designed a special measurement geometry to measure the resistance and found that single-crystal Bi2Te2Se exhibits a crossover from bulk to surface conduction at 20 K. Simultaneously, the material also shows strong evidence of weak antilocalization in magnetotransport owing to the protection against scattering by conducting surface states. This simple geometry facilitates finding evidence of surface transport in topological insulators, which are promising materials for future spintronic applications.

Ternary semiconducting or metallic half-Heusler compounds with an atomic composition 1:1:1 are widely studied for their flexible electronic properties and functionalities. Recently, a new material property of half-Heusler compounds was predicted based on electronic structure calculations: the topological insulator. In topological insulators, the metallic surface states are protected from impurity backscattering due to spin-momentum locking. This opens up new perspectives in engineering multifunctional materials. In this article, we introduce half-Heusler materials from the crystallographic and electronic structure point of view. We present an effective model Hamiltonian from which the topological state can be derived, notably from a non-trivial inverted band structure. We discuss general implications of the inverted band structure with a focus on the detection of the topological surface states in experiments by reviewing several exemplary materials. Special attention is given to superconducting half-Heusler materials, which have attracted ample attention as a platform for non-centrosymmetric and topological superconductivity.

The topological surface states of mercury telluride (HgTe) are studied by ab initio calculations assuming different strains and surface terminations. For the Te-terminated surface, a single Dirac cone exists at the Γ-point. The Dirac point shifts up from the bulk valence bands into the energy gap when the substrate-induced strain increases. At the experimental strain value (0.3%), the Dirac point lies slightly below the bulk valence band maximum. A left-handed spin texture was observed in the upper Dirac cone, similar to that of the Bi₂Se₃-type topological insulator. For the Hg-terminated surface, three Dirac cones appear at three time-reversal-invariant momenta, excluding the Γ-point, with non-trivial spin textures.

Developing graphene-based nanoelectronics hinges on opening a band gap in the electronic structure of graphene, which is commonly achieved by breaking the inversion symmetry of the graphene lattice via an electric field (gate bias) or asymmetric doping of graphene layers. Here we introduce a new design strategy that places a bilayer graphene sheet sandwiched between two cladding layers of materials that possess strong spin-orbit coupling (e.g., Bi₂Te ₃). Our ab initio and tight-binding calculations show that a proximity enhanced spin-orbit coupling effect opens a large (44 meV) band gap in bilayer graphene without breaking its lattice symmetry, and the band gap can be effectively tuned by an interlayer stacking pattern and significantly enhanced by interlayer compression. The feasibility of this quantum-well structure is demonstrated by recent experimental realization of high-quality heterojunctions between graphene and Bi₂Te₃, and this design also conforms to existing fabrication techniques in the semiconductor industry. The proposed quantum-well structure is expected to be especially robust since it does not require an external power supply to open and maintain a band gap, and the cladding layers provide protection against environmental degradation of the graphene layer in its device applications.

Magnetic properties and spin dynamics have been studied for the structurally ordered double perovskite Sr2CoOsO6. Neutron diffraction, muon-spin relaxation, and ac-susceptibility measurements reveal two antiferromagnetic (AFM) phases on cooling from room temperature down to 2 K. In the first AFM phase, with transition temperature TN1=108K, cobalt (3d7, S=3/2) and osmium (5d2, S=1) moments fluctuate dynamically, while their average effective moments undergo long-range order. In the second AFM phase below TN2=67K, cobalt moments first become frozen and induce a noncollinear spin-canted AFM state, while dynamically fluctuating osmium moments are later frozen into a randomly canted state at T≈5K. Ab initio calculations indicate that the effective exchange coupling between cobalt and osmium sites is rather weak, so that cobalt and osmium sublattices exhibit different ground states and spin dynamics, making Sr2CoOsO6 distinct from previously reported double-perovskite compounds.

Based on first-principles calculations, we predict Bi2TeI, a stoichiometric compound that is synthesized, to be a weak topological insulator (TI) in layered subvalent bismuth telluroiodides. Within a bulk energy gap of 80 meV, two Dirac-cone-like topological surface states exist on the side surface perpendicular to the BiTeI layer plane. These Dirac cones are relatively isotropic due to the strong interlayer coupling, distinguished from those of previously reported weak TI candidates. Moreover, with chemically stable cladding layers, the BiTeI-Bi2-BiTeI sandwiched structure is a robust quantum spin Hall system, which can be obtained by simply cleaving the bulk Bi2TeI.

The surface band bending tunes considerably the surface band structures and transport properties in topological insulators. We present a direct measurement of the band bending on the Bi₂Se₃ by using the bulk sensitive angular-resolved hard x-ray photospectroscopy (HAXPES). We tracked the depth dependence of the energy shift of Bi and Se core states. We estimate that the band bending extends up to about 20 nm into the bulk with an amplitude of 0.23-0.26 eV, consistent with profiles previously deduced from the binding energies of surface states in this material.

Topological insulators are a new class of quantum materials that are characterized by robust topological surface states (TSSs) inside the bulk insulating gap, which hold great potential for applications in quantum information and spintronics as well as thermoelectrics. One major obstacle is the relatively small size of the bulk bandgap, which is typically around 0.3 eV for the known topological insulator materials (ref.and references therein). Here we demonstrate through ab initio calculations that a known superconductor BaBiO 3 (BBO) with a T c of nearly 30 K (refs,) emerges as a topological insulator in the electron-doped region. BBO exhibits a large topological energy gap of 0.7 eV, inside which a Dirac type of TSSs exists. As the first oxide topological insulator, BBO is naturally stable against surface oxidization and degradation, distinct from chalcogenide topological insulators. An extra advantage of BBO lies in its ability to serve as an interface between TSSs and superconductors to realize Majorana fermions for future applications in quantum computation.

The search for large-gap quantum spin Hall (QSH) insulators and effective approaches to tune QSH states is important for both fundamental and practical interests. Based on first-principles calculations we find two-dimensional tin films are QSH insulators with sizable bulk gaps of 0.3 eV, sufficiently large for practical applications at room temperature. These QSH states can be effectively tuned by chemical functionalization and by external strain. The mechanism for the QSH effect in this system is band inversion at the Gamma point, similar to the case of a HgTe quantum well. With surface doping of magnetic elements, the quantum anomalous Hall effect could also be realized.

We investigate the structural stability and magnetic properties of the cubic, tetragonal and hexagonal phases of Mn₃Z (Z=Ga, Sn and Ge) Heusler compounds using first-principles density-functional theory. We propose that the cubic phase plays an important role as an intermediate state in the phase transition from the hexagonal to the tetragonal phases. Consequently, Mn₃Ga and Mn₃Ge behave differently from Mn₃Sn, because the relative energies of the cubic and hexagonal phases are different. This result agrees with experimental observations for these three compounds. The weak ferromagnetism of the hexagonal phase and the perpendicular magnetocrystalline anisotropy of the tetragonal phase obtained in our calculations are also consistent with experiment.

In Dirac materials, like graphene or topological insulators, massless pseudorelativistic electrons promise new, very fast electronic devices by utilizing the partial suppression of backscattering. However, the semimetal nature of graphene makes the realization of practical field effect transistors difficult, due to small on-off current ratios. Here, we propose a new concept, based on Dirac states inside the conduction (or valence) band of a lightly doped wide band gap semiconductor. With the application of a gate voltage, the Dirac states become populated; that is, the Fermi level is switched between the "classical" high-resistivity semiconducting and the relativistic high-mobility metallic range. We demonstrate by theoretical calculations that such a transition can be realized, for example, in thin anatase nanowires, which have been synthesized before. Ta-doped anatase nanowires offer an excellent possibility to build field effect transistors with high speed and good on-off ratio. Guidelines for finding similar "Dirac semiconductors" are provided.

Topological insulators (TIs) are a new quantum state of matter which have gapless surface states inside the bulk energy gap [1-4]. Starting with the discovery of two-dimensional TIs, the HgTe-based quantum wells [5, 6], many new topological materials have been theoretically predicted and experimentally observed. Currently known TI materials can possibly be classified into two families [7], the HgTe family and the Bi₂Se₃ family. The signatures found in the electronic structure of a TI also cause these materials to be excellent thermoelectric materials [8-10]. On the other hand, excellent thermoelectric materials can be also topologically trivial. Here we present a short introduction to topological insulators and thermoelectrics, and give examples of compound classes where both good thermoelectric properties and topological insulators can be found.

A phosphorus (P) donor has been extensively studied in bulk Si to realize the concept of Kane quantum computers. In most cases the quantum bit was realized as an entanglement between the donor electron spin and the nonzero nuclei spin of the donor impurity mediated by the hyperfine coupling between them. The donor ionization energies and the spin-lattice relaxation time limited the temperatures to a few kelvin in these experiments. Here, we demonstrate by means of ab initio density functional theory calculations that quantum confinement in thin Si nanowires (SiNWs) results in (i) larger excitation energies of donor impurity and (ii) a sensitive manipulation of the hyperfine coupling by external electric field. We propose that these features may allow to realize the quantum bit (qubit) experiments at elevated temperatures with a strength of electric fields applicable in current field-effect transistor technology. We also show that the strength of quantum confinement and the presence of strain induced by the surface termination may significantly affect the ground and excited states of the donors in thin SiNWs, possibly allowing an optical read-out of the electron spin.

Recently, topological insulator materials have been theoretically predicted and experimentally observed in both 2D and 3D systems. We first review the basic models and physical properties of topological insulators, using HgTe and Bi ₂Se ₃ as prime examples. We then give a comprehensive survey of topological insulators which have been predicted so far, and discuss the current experimental status.

Due to the proximity to an embedding medium with low dielectric constant (e.g., oxides), semiconductor nanowires have higher impurity ionization energy than their bulk counterparts, resulting lower free carrier density. Using ab initio calculations within density functional theory, we propose a way to reduce the ionization energy in nanowires by fabricating a special cross section with appropriate engineering of doping and an applied gate voltage. We demonstrate on a phosphorus-doped silicon nanowire that the ionization energy can be effectively tuned and the impurity backscattering can also be reduced. For instance, even without special engineering of doping, the free carrier density may increase by 40% in a silicon nanowire with 15 nm diameter and special cross section. Our proposal has profound implications to fabricate nanowire devices with high carrier density.

Surface motion of a topological defect between p (2 × 2) and c (4 × 2) structures, a "kink", across buckled Sn-Ge and Si-Ge dimers on Ge(0 0 1) surfaces was investigated using scanning tunneling microscopy. Energy thresholds of π^* electrons for flipping these dimers in the kink are obtained by analyzing the kink surface motion. Electronic states of these systems and energy barriers for flipping the dimers are examined by first-principles calculations for considering elementary processes of the electronically-excited flip motion of the dimers. We propose that the flip motion is caused by a resonant scattering of the π^* electrons with localized electronic states at the kink.

Scattering potentials for π electrons at Si-Ge and Sn-Ge dimers on a Ge(001) surface are studied by scanning tunneling microscopy and ab initio calculations. Phase-shift analysis of standing waves in dI/dV images reveals that Si and Sn atoms located in the conduction path of π electrons form potentials with the sign opposite to each other. Density-functional calculations and simple calculations based on the nearly-free-electron model explain the observed potential structures. These results are qualitatively understood by relative p -orbital energy of the Si, Sn, and Ge atoms.