Publications

The multiband kagome superconductor CsV3Sb5 exhibits complex orbital textures on the Fermi surface, making the orbital origins of its cascade of correlated electronic states and superconductivity a major scientific puzzle. Chemical doping of the kagome plane can simultaneously tune the exotic states and the Fermi-surface orbital texture and thus offers a unique opportunity to correlate the given states with specific orbitals. In this Letter, by substituting V atoms with Ti in the kagome superconductor CsV3Sb5, we reveal the orbital origin of a cascade of its correlated electronic states through the orbital-resolved quasiparticle interference. We analyze the quasiparticle interference changes associated with different orbitals, aided by first-principles calculations. We have observed that the in-plane and out-of-plane vanadium 3d orbitals cooperate to form unidirectional coherent states in pristine CsV3Sb5, whereas the out-of-plane component disappears with doping-induced suppression of charge density wave and global electronic nematicity. In addition, the Sb pz orbital plays an important role in both the pseudogap and superconducting states in CsV3Sb5. Our findings offer new insights into multiorbital physics in quantum materials that are generally manifested with intriguing correlations between atomic orbitals and symmetry-encoded correlated electronic states.

Electrical magnetochiral anisotropy (EMCA) refers to the chirality- and current-dependent nonlinear magnetoresistance in chiral conductors and is commonly interpreted in a semiclassical picture. In this work, we reveal a quantum geometry origin of EMCA using a chiral rectangular lattice model that resembles a chiral organic conductor (DM-EDT-TTF) 2 ClO 4 studied for EMCA recently and exhibits symmetry-protected Dirac bands similar to those of graphene. Compared to the semiclassical term, we find that Dirac states contribute significantly to both traditional longitudinal EMCA and the unconventional transverse EMCA via the quantum metric when Fermi energy is close to the Dirac point. Besides, we discover that a topological insulator state can emerge once spin-orbit coupling is added to our chiral model lattice. Our work paves a path toward understanding quantum geometry in the magnetotransport of chiral materials.

The exploration of magnetic topological insulators is instrumental in exploring axion electrodynamics and intriguing transport phenomena, such as the quantum anomalous Hall effect. Here, we report that a family of magnetic compounds Eu2n+1In2(As,Sb)2n+2 (n=0,1,2) exhibit both gapless Dirac surface states and chiral hinge modes. Such a hybrid-order topology hatches surface-dependent quantum geometry. By mapping the responses into real space, we demonstrate the existence of chiral hinge modes along the c direction, which originate from the half-quantized anomalous Hall effect on two gapped ac/bc facets due to Berry curvature, while the unpinned Dirac surface states on the gapless ab facet generate an intrinsic nonlinear anomalous Hall effect due to the quantum metric. When Eu3In2As4 is polarized to the ferromagnetic phase by an external magnetic field, it becomes an ideal Weyl semimetal with a single pair of type-I Weyl points and no extra Fermi pocket. Our work predicts rich topological states sensitive to magnetic structures, quantum geometry-induced transport, and topological superconductivity if proximitized with a superconductor.

In the presence of a high magnetic field, quantum Hall systems usually host both even- and odd-integer quantized states because of lifted band degeneracies. Selective control of these quantized states is challenging but essential to understand the exotic ground states and manipulate the spin textures. Here we demonstrate the quantum Hall effect in Bi₂O₂Se thin films. In magnetic fields as high as 50 T, we observe only even-integer quantum Hall states, but there is no sign of odd-integer states. However, when reducing the thickness of the epitaxial Bi₂O₂Se film to one unit cell, we observe both odd- and even-integer states in this Janus (asymmetric) film grown on SrTiO₃. By means of a Rashba bilayer model based on the ab initio band structures of Bi₂O₂Se thin films, we can ascribe the only even-integer states in thicker films to the hidden Rasbha effect, where the local inversion-symmetry breaking in two sectors of the [Bi₂O₂]²⁺ layer yields opposite Rashba spin polarizations, which compensate with each other. In the one-unit-cell Bi₂O₂Se film grown on SrTiO₃, the asymmetry introduced by the top surface and bottom interface induces a net polar field. The resulting global Rashba effect lifts the band degeneracies present in the symmetric case of thicker films.

Two-dimensional semiconductors present unique opportunities to intertwine optical and magnetic functionalities and to tune these performances through defects and dopants. Here, we integrate exciton pumping into a quantum sensing protocol on nitrogen-vacancy centers in diamond to image the optically induced transient stray fields in few-layer, antiferromagnetic CrCl3. We discover that exciton recombination enhances the in-plane magnetization of the CrCl3 layers, with a predominant effect in the surface monolayers. Concomitantly, time-resolved photoluminescence measurements reveal that nonradiative exciton recombination intensifies in atomically thin CrCl3 with tightly localized, nearly dipole-forbidden excitons and amplified surface-to-volume ratio. Supported by experiments under controlled surface exposure and density functional theory calculations, we interpret the magnetically enhanced state to result from a defect-assisted Auger recombination that optically activates electron transfer between water vapor related surface impurities and the spin-polarized conduction band. Our work validates defect engineering as a route to enhance intrinsic magnetism in single magnetic layers and opens an experimental platform for studying optically induced, transient magnetism in condensed matter systems.

Magnetic kagome materials provide a fascinating playground for exploring the interplay of magnetism, correlation and topology. Many magnetic kagome systems have been reported including the binary FemXn (X=Sn, Ge; m:n=3:1, 3:2, 1:1) family and the rare earth RMn6Sn6 (R=rare earth) family, where their kagome flat bands are calculated to be near the Fermi level in the paramagnetic phase. While partially filling a kagome flat band is predicted to give rise to a Stoner-type ferromagnetism, experimental visualization of the magnetic splitting across the ordering temperature has not been reported for any of these systems due to the high ordering temperatures, hence leaving the nature of magnetism in kagome magnets an open question. Here, we probe the electronic structure with angle-resolved photoemission spectroscopy in a kagome magnet thin film FeSn synthesized using molecular beam epitaxy. We identify the exchange-split kagome flat bands, whose splitting persists above the magnetic ordering temperature, indicative of a local moment picture. Such local moments in the presence of the topological flat band are consistent with the compact molecular orbitals predicted in theory. We further observe a large spin-orbital selective band renormalization in the Fe formula presented spin majority channel reminiscent of the orbital selective correlation effects in the iron-based superconductors. Our discovery of the coexistence of local moments with topological flat bands in a kagome system echoes similar findings in magic-angle twisted bilayer graphene, and provides a basis for theoretical effort towards modeling correlation effects in magnetic flat band systems.

In chemistry and biochemistry, chirality represents the structural asymmetry characterized by nonsuperimposable mirror images for a material such as DNA. In physics, however, chirality commonly refers to the spinmomentum locking of a particle or quasiparticle in the momentum space. While seemingly disconnected, structural chirality in molecules and crystals can drive electronic chirality through orbitalmomentum locking; that is, chirality can be transferred from the atomic geometry to electronic orbitals. Electronic chirality provides an insightful understanding of chirality-induced spin selectivity, in which electrons exhibit salient spin polarization after going through a chiral material, and electrical magnetochiral anisotropy, which is characterized by diode-like transport. It further gives rise to new phenomena, such as anomalous circularly polarized light emission, in which the light handedness relies on the emission direction. These chirality-driven effects will generate broad impacts for fundamental science and technology applications in spintronics, optoelectronics, and biochemistry.

It is well known that the anomalous Hall effect displayed in ferromagnets is much stronger than the ordinary Hall effect. Similarly, the magneto-optical Kerr effect (MOKE) is orders of magnitude stronger than the optical Hall effect taking place in normal metals. Here, we present a MOKE technique that we term the 'Ferris' MOKE which is based on large-amplitude modulation of the externally applied magnetic field such that the sensitivity is enhanced by more than an order of magnitude. Consequently, the Ferris MOKE is found suitable for measurement of the optical Hall effect at visible light wavelengths where the effective electrical displacement is short. We derive a model that builds on the Lorentz-Drude formalism that accounts for the evanescent waves in the metal. By complementing the measurements with carrier density data extracted by DC Hall measurements, we show that the 'Ferris MOKE' measurement can reproduce previously reported effective masses that is indicative of the effective band curvature. Since the optical cycle is much shorter than the Drude mean free path, the technique may prove useful for probing intrinsic properties of the band structure and topological states of matter in non-magnetic materials.

Electrical generation and transduction of polarized electron spins in semiconductors (SCs) are of central interest in spintronics and quantum information science. While spin generation in SCs is frequently realized via electrical injection from a ferromagnet (FM), there are significant advantages in nonmagnetic pathways of creating spin polarization. One such pathway exploits the interplay of electron spin with chirality in electronic structures or real space. Here, utilizing chirality-induced spin selectivity (CISS), the efficient creation of spin accumulation in n-doped GaAs via electric current injection from a normal metal (Au) electrode through a self-assembled monolayer (SAM) of chiral molecules (α-helix l-polyalanine, AHPA-L), is demonstrated. The resulting spin polarization is detected as a Hanle effect in the n-GaAs, which is found to obey a distinct universal scaling with temperature and bias current consistent with chirality-induced spin accumulation. The experiment constitutes a definitive observation of CISS in a fully nonmagnetic device structure and demonstration of its ability to generate spin accumulation in a conventional SC. The results thus place key constraints on the physical mechanism of CISS and present a new scheme for magnet-free SC spintronics.

The so-called \u201cextreme magnetoresistance\u201d (XMR) found in few conductors poses interesting conceptual challenges which address needs in technology. In contrast to the more common XMR in semi-metals, PtSn₄ stands out as a rare example of a high carrier density multi-band metal exhibiting XMR, sparking an active debate about its microscopic origin. Here we report a sharp sensitivity of its XMR upon the field angle, with an almost complete collapse only for one specific current and field direction (B//b, I//a). Corroborated by band-structure calculations, we identify a singular open orbit on one of its Fermi surface sheets as the origin of this collapse. This remarkably switchable XMR resolves the puzzle in PtSn₄ as a semi-classical effect of an ultra-pure, compensated carrier metal. It further showcases the importance of Ockhams razor in uncommon magnetotransport phenomena and demonstrates the remarkable physical properties conventional metals can exhibit given they are superbly clean.

Rare-earth monopnictides are a family of materials simultaneously displaying complex magnetism, strong electronic correlation, and topological band structure. The recently discovered emergent arc-like surface states in these materials have been attributed to the multi-wave-vector antiferromagnetic order, yet the direct experimental evidence has been elusive. Here we report observation of non-collinear antiferromagnetic order with multiple modulations using spin-polarized scanning tunneling microscopy. Moreover, we discover a hidden spin-rotation transition of single-to-multiple modulations 2K below the Néel temperature. The hidden transition coincides with the onset of the surface states splitting observed by our angle-resolved photoemission spectroscopy measurements. Single modulation gives rise to a band inversion with induced topological surface states in a local momentum region while the full Brillouin zone carries trivial topological indices, and multiple modulation further splits the surface bands via non-collinear spin tilting, as revealed by our calculations. The direct evidence of the non-collinear spin order in NdSb not only clarifies the mechanism of the emergent topological surface states, but also opens up a new paradigm of control and manipulation of band topology with magnetism.

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.]

The combination of a geometrically frustrated lattice, and similar energy scales between degrees of freedom endows two-dimensional Kagome metals with a rich array of quantum phases and renders them ideal for studying strong electron correlations and band topology. The Kagome metal, FeGe is a noted example of this, exhibiting A-type collinear antiferromagnetic (AFM) order at T_N ≈ 400 K, then establishes a charge density wave (CDW) phase coupled with AFM ordered moment below T_CDW ≈ 110 K, and finally forms a c-axis double cone AFM structure around T_Canting ≈ 60 K. Here we use neutron scattering to demonstrate the presence of gapless incommensurate spin excitations associated with the double cone AFM structure of FeGe at temperatures well above T_Canting and T_CDW that merge into gapped commensurate spin waves from the A-type AFM order. Commensurate spin waves follow the Bose factor and fit the Heisenberg Hamiltonian, while the incommensurate spin excitations, emerging below T_N where AFM order is commensurate, start to deviate from the Bose factor around T_CDW, and peaks at T_Canting. This is consistent with a critical scattering of a second order magnetic phase transition with decreasing temperature. By comparing these results with density functional theory calculations, we conclude that the incommensurate magnetic structure arises from the nested Fermi surfaces of itinerant electrons and the formation of a spin density wave order.

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.

Nontrivial electronic states are attracting intense attention in low-dimensional physics. Though chirality has been identified in charge states with a scalar order parameter, its intertwining with charge density waves (CDW), film thickness, and the impact on the electronic behaviors remain less well understood. Here, using scanning tunneling microscopy, we report a 2 × 2 chiral CDW as well as a strong suppression of the Te-5p hole-band backscattering in monolayer 1T-TiTe₂. These exotic characters vanish in bilayer TiTe₂ in a non-CDW state. Theoretical calculations prove that chirality comes from a helical stacking of the triple-q CDW components and, therefore, can persist at the two-dimensional limit. Furthermore, the chirality renders the Te-5p bands with an unconventional orbital texture that prohibits electron backscattering. Our study establishes TiTe₂ as a promising playground for manipulating the chiral ground states at the monolayer limit and provides a novel path to engineer electronic properties from an orbital degree.

Kagome metals are topological materials with a rich phase diagram featuring various charge density wave orders and even unconventional superconductivity. However, little is still known about possible spin polarized responses in these nonmagnetic compounds. Here, we perform ab initio calculations of the intrinsic spin Hall effect (SHE) in the kagome metals AV3Sb5 (A=Cs, Rb, K), CsTi3Bi5, and ScV6Sn6. We report large spin Hall conductivities, comparable with the Weyl semimetal TaAs. Additionally, in CsV3Sb5 the SHE is strongly renormalized by the charge density wave order. We can understand these results based on the topological properties of band structures, demonstrating that the SHE is dominated by the position and shape of the Dirac nodal lines in the kagome sublattice. Our results suggest kagome materials as a promising, tunable platform for future spintronics applications.

A recently discovered group of kagome metals AV3Sb5 (A = K, Rb, Cs) exhibit a variety of intertwined unconventional electronic phases, which emerge from a puzzling charge density wave phase. Understanding of this charge-ordered parent phase is crucial for deciphering the entire phase diagram. However, the mechanism of the charge density wave is still controversial, and its primary source of fluctuations-the collective modes-has not been experimentally observed. Here, we use ultrashort laser pulses to melt the charge order in CsV3Sb5 and record the resulting dynamics using femtosecond angle-resolved photoemission. We resolve the melting time of the charge order and directly observe its amplitude mode, imposing a fundamental limit for the fastest possible lattice rearrangement time. These observations together with ab initio calculations provide clear evidence for a structural rather than electronic mechanism of the charge density wave. Our findings pave the way for a better understanding of the unconventional phases hosted on the kagome lattice.

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.

Chirality has been a property of central importance in physics, chemistry and biology for more than a century. Recently, electrons were found to become spin polarized after transmitting through chiral molecules, crystals, and their hybrids. This phenomenon, called chirality-induced spin selectivity (CISS), presents broad application potentials and far-reaching fundamental implications involving intricate interplays among structural chirality, topological states, and electronic spin and orbitals. However, the microscopic picture of how chiral geometry influences electronic spin remains elusive, given the negligible spin-orbit coupling (SOC) in organic molecules. In this work, we address this issue via a direct comparison of magnetoconductance (MC) measurements on magnetic semiconductor-based chiral molecular spin valves with normal metal electrodes of contrasting SOC strengths. The experiment reveals that a heavy-metal electrode provides SOC to convert the orbital polarization induced by the chiral molecular structure to spin polarization. Our results illustrate the essential role of SOC in the metal electrode for the CISS spin valve effect. A tunneling model with a magnetochiral modulation of the potential barrier is shown to quantitatively account for the unusual transport behavior.

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 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.

Kagome materials are emerging platforms for studying charge and spin orders. In this Letter, we have revealed a rich lattice instability in a Z₂ kagome metal ScV₆Sn₆ by first-principles calculations. Beyond verifying the √3×√3×3 charge density wave (CDW) order observed by the recent experiment, we further identified three more possible CDW structures, i.e., √3×√3×2 CDW with P6/mmm symmetry, 2×2×2 CDW with Immm symmetry, and 2×2×2 CDW with P6/mmm symmetry. The former two are more energetically favored than the √3×√3×3 phase, while the third one is comparable in energy. These CDW distortions involve mainly out-of-plane motions of Sc and Sn atoms, while V atoms constituting the kagome net are almost unchanged. We attribute the lattice instability to the smallness of Sc atomic radius. In contrast, such instability disappears in its sister compounds RV₆Sn₆ (R is Y, or a rare-earth element), which exhibit quite similar electronic band structures to the Sc compound, because R has a larger atomic radius. Our work indicates that ScV₆Sn₆ might exhibit varied CDW phases in different experimental conditions and provides insights to explore rich charge orders in kagome materials.

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.

Electron hydrodynamics typically emerges in electron fluids with a high electronelectron collision rate. However, new experiments with thin flakes of WTe₂ have revealed that other momentum-conserving scattering processes can replace the role of the electronelectron interaction, thereby leading to a novel, so-called para-hydrodynamic regime. Here, we develop the kinetic theory for para-hydrodynamic transport. To this end, we consider a ballistic electron gas in a thin three-dimensional sheet where the momentum-relaxing (lmr) and momentum-conserving (lmc) mean free paths are decreased due to boundary scattering from a rough surface. The resulting effective mean free path of the in-plane components of the electronic flow is then expressed in terms of microscopic parameters of the sheet boundaries, predicting that a para-hydrodynamic regime with lmr ≫ lmc emerges generically in ultraclean three-dimensional materials. Using our approach, we recover the transport properties of WTe₂ in the para-hydrodynamic regime in good agreement with existing experiments.

Many experiments observed a metallic behavior at zero magnetic fields (antiferromagnetic phase, AFM) in MnBi₂Te₄ thin film transport, which coincides with gapless surface states observed by angle-resolved photoemission spectroscopy, while it can become a Chern insulator at field larger than 6 T (ferromagnetic phase, FM). Thus, the zero-field surface magnetism was once speculated to be different from the bulk AFM phase. However, recent magnetic force microscopy refutes this assumption by detecting persistent AFM order on the surface. In this Letter, we propose a mechanism related to surface defects that can rationalize these contradicting observations in different experiments. We find that co-antisites (exchanging Mn and Bi atoms in the surface van der Waals layer) can strongly suppress the magnetic gap down to several meV in the AFM phase without violating the magnetic order but preserve the magnetic gap in the FM phase. The different gap sizes between AFM and FM phases are caused by the exchange interaction cancellation or collaboration of the top two van der Waals layers manifested by defect-induced surface charge redistribution among the top two van der Waals layers. This theory can be validated by the position- and field-dependent gap in future surface spectroscopy measurements. Our work suggests suppressing related defects in samples to realize the quantum anomalous Hall insulator or axion insulator at zero fields.

Chiral circularly polarized (CP) light is central to many photonic technologies, from the optical communication of spin information to novel display and imaging technologies. As such, there has been significant effort in the development of chiral emissive materials that enable the emission of strongly dissymmetric CP light from organic light-emitting diodes (OLEDs). It has been widely accepted that the molecular chirality of the active layer determines the favoured light handedness of the CP emission in such devices, regardless of the light-emitting direction. Here we discover that, unconventionally, oppositely propagating CP light exhibits opposite handedness, and reversing the current flow in OLEDs also switches the handedness of the emitted CP light. This direction-dependent CP emission boosts the net polarization rate by orders of magnitude by resolving an established issue in CP-OLEDs, where the CP light reflected by the back electrode typically erodes the measured dissymmetry. Through detailed theoretical analysis, we assign this anomalous CP emission to a ubiquitous topological electronic property in chiral materials, namely orbitalmomentum locking. Our work paves the way to design new chiroptoelectronic devices and probes the close connections between chiral materials, topological electrons and CP light in the quantum regime.

The invention of scanning probe microscopy revolutionized the way electronic phenomena are visualized1. Whereas present-day probes can access a variety of electronic properties at a single location in space2, a scanning microscope that can directly probe the quantum mechanical existence of an electron at several locations would provide direct access to key quantum properties of electronic systems, so far unreachable. Here, we demonstrate a conceptually new type of scanning probe microscopethe quantum twisting microscope (QTM)capable of performing local interference experiments at its tip. The QTM is based on a unique van der Waals tip, allowing the creation of pristine two-dimensional junctions, which provide a multitude of coherently interfering paths for an electron to tunnel into a sample. With the addition of a continuously scanned twist angle between the tip and sample, this microscope probes electrons along a line in momentum space similar to how a scanning tunnelling microscope probes electrons along a line in real space. Through a series of experiments, we demonstrate room-temperature quantum coherence at the tip, study the twist angle evolution of twisted bilayer graphene, directly image the energy bands of monolayer and twisted bilayer graphene and, finally, apply large local pressures while visualizing the gradual flattening of the low-energy band of twisted bilayer graphene. The QTM opens the way for new classes of experiments on quantum materials.

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 flavour 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=1, we observe a zero-field Chern insulator, whichrather than being described by a global topologically invariant Cforms a mosaic of microscopic patches of C=−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, 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 WiedemannFranz 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 electronelectron 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 lightmatter 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 rates²⁷. 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 lightmatter interaction induces notable modifications to the electronic and optical properties⁸¹⁰, 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 fields 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 lightmatter interactions in strongly driven crystals and the sub-cycle modifications in their effective band structure.

Magnetic topological insulators (MnBi₂Te₄)(Bi₂Te₃)_n (n=0,1,2,3) are promising to realize exotic topological states such as the quantum anomalous Hall effect (QAHE) and axion insulator (AI), where the Bi₂Te₃ layer introduces versatility to engineer electronic and magnetic properties. However, whether surface states on the Bi₂Te₃ terminated facet are gapless or gapped is debated, and its consequences in thin-film properties are rarely discussed. In this work, we find that the Bi₂Te₃ terminated facets are gapless for n≥1 compounds by calculations. Although the surface Bi₂Te₃ (one layer or more) and underlying MnBi₂Te₄ layers hybridize and give rise to a gap, such a hybridization gap may overlap with bulk valence bands, leading to a gapless surface after all. Such a metallic surface poses a fundamental challenge to realize QAHE or AI, which requires an insulating gap in thin films with at least one Bi₂Te₃ surface. In theory, the insulating phase can still be realized in a film if both surfaces are MnBi₂Te₄ layers. Otherwise, it requires that the film thickness be less than 10-20nm to push down bulk valence bands via the size effect. Our work paves the way to understand surface states and design bulk-insulating quantum devices in magnetic topological materials.

A critical overview of the theory of the chirality-induced spin selectivity (CISS) effect, that is, phenomena in which the chirality of molecular species imparts significant spin selectivity to various electron processes, is provided. Based on discussions in a recently held workshop, and further work published since, the status of CISS effects-in electron transmission, electron transport, and chemical reactions-is reviewed. For each, a detailed discussion of the state-of-the-art in theoretical understanding is provided and remaining challenges and research opportunities are identified.

Kagome metal TbMn6Sn6 was recently discovered to be a ferrimagnetic topological Dirac material by scanning tunneling microscopy/spectroscopy measurements. Here, we report the observation of large anomalous Nernst effect and anomalous thermal Hall effect in this compound. The anomalous transverse transport is consistent with the Berry curvature contribution from the massive Dirac gaps in the 3D momentum space as demonstrated by our first-principles calculations. Furthermore, the transverse thermoelectric transport exhibits asymmetry with respect to the applied magnetic field, i.e., an exchange-bias behavior. Together, these features place TbMn6Sn6 as a promising system for the outstanding thermoelectric performance based on anomalous Nernst effect.

The transition metal kagome lattice materials host frustrated, correlated and topological quantum states of matter¹⁹. Recently, a new family of vanadium-based kagome metals, AV₃Sb₅ (A = K, Rb or Cs), with topological band structures has been discovered^10,11. These layered compounds are nonmagnetic and undergo charge density wave transitions before developing superconductivity at low temperatures¹¹¹⁹. Here we report the observation of unconventional superconductivity and a pair density wave (PDW) in CsV₃Sb₅ using scanning tunnelling microscope/spectroscopy and Josephson scanning tunnelling spectroscopy. We find that CsV₃Sb₅ exhibits a V-shaped pairing gap Δ ~ 0.5 meV and is a strong-coupling superconductor (2Δ/k_BT_c ~ 5) that coexists with 4a₀ unidirectional and 2a₀ × 2a₀ charge order. Remarkably, we discover a 3Q PDW accompanied by bidirectional 4a₀/3 spatial modulations of the superconducting gap, coherence peak and gap depth in the tunnelling conductance. We term this novel quantum state a roton PDW associated with an underlying vortexantivortex lattice that can account for the observed conductance modulations. Probing the electronic states in the vortex halo in an applied magnetic field, in strong field that suppresses superconductivity and in zero field above T_c, reveals that the PDW is a primary state responsible for an emergent pseudogap and intertwined electronic order. Our findings show striking analogies and distinctions to the phenomenology of high-T_c cuprate superconductors, and provide groundwork for understanding the microscopic origin of correlated electronic states and superconductivity in vanadium-based kagome metals.

We use spin torque ferromagnetic resonance and ferromagnetic-resonance-driven spin pumping to detect spin-charge interconversion at room temperature in heterostructure devices that interface an archetypal Dirac semimetal, Cd3As2, with a metallic ferromagnet, Ni0.80Fe0.20 (permalloy). Angle-resolved photoemission directly reveals the Dirac-semimetal nature of the samples prior to device fabrication and high-resolution transmission electron microscopy is used to characterize the crystalline structure and the relevant heterointerfaces. We find that the spin-charge interconversion efficiency in Cd3As2/permalloy heterostructures is comparable to that in heavy metals and that it is enhanced by the presence of an interfacial oxide. Spin torque ferromagnetic resonance measurements reveal an in-plane spin polarization regardless of an oxidized or pristine interface. We discuss the underlying mechanisms for spin-charge interconversion by comparing our results with first principles calculations and conclude that extrinsic mechanisms dominate the observed phenomena. Our results indicate a need for caution in interpretations of spin-transport and spin-charge conversion experiments in Cd3As2 devices that seek to invoke the role of topological Dirac and Fermi arc states.

Co3Sn2S2 is a ferromagnetic semi-metal with Weyl nodes in its band structure and a large anomalous Hall effect below its Curie temperature of 177 K. We present a detailed study of its Fermi surface and examine the relevance of the anomalous transverse Wiedemann Franz law to it. We studied Shubnikov-de Haas oscillations along two orientations in single crystals with a mobility as high as 2.7×103 cm2 V-1 s-1 subject to a magnetic field as large as ∼60 T. The angle dependence of the frequencies is comparable with density functional theory (DFT) calculations and reveals two types of hole pockets (H1, H2) and two types of electron pockets (E1, E2). An additional unexpected frequency emerges at high magnetic field. We attribute it to magnetic breakdown between the hole pocket H2 and the electron pocket E2, since it is close to the sum of the E2 and H2 fundamental frequencies. By measuring the anomalous thermal and electrical Hall conductivities, we quantified the anomalous transverse Lorenz ratio, which is close to the Sommerfeld ratio (L_0 = 1/2π k_B2e2) below 100 K and deviates downwards at higher temperatures. This finite temperature deviation from the anomalous Wiedemann-Franz law is a source of information on the distance between the sources and sinks of the Berry curvature and the chemical potential.

The classic magnetic induction effect is usually considered in electric circuits or conductor coils. In this work, we propose quantum induction effects induced by the Berry curvature in homogenous solids. Two different types of quantum inductions are identified in the higher order of a magnetic field. They are closely related to the magnetic-field-induced anomalous velocityproportional to the Berry curvature so that both quantum inductions become significantly enhanced near Weyl points. Further, we propose an ac-magnetic-field measurement to detect quantum induction effects and distinguish them from classical induction.

Kagome metals AV3Sb5 (A=K, Rb, and Cs) exhibit intriguing superconductivity below 0.9∼2.5 K, a charge density wave (CDW) transition around 80∼100 K, and Z2 topological surface states. The nature of the CDW phase and its relation to superconductivity remains elusive. In this work, we investigate the electronic and structural properties of CDW by first-principles calculations. We reveal an inverse Star of David deformation as the 2×2×2 CDW ground state of the kagome lattice. The kagome lattice shows softening breathing-phonon modes, indicating the structural instability. However, electrons play an essential role in the CDW transition via Fermi surface nesting and van Hove singularity. The inverse Star of David structure agrees with recent experiments by scanning tunneling microscopy (STM). The CDW phase inherits the nontrivial Z2-type topological band structure. Further, we find that the electron-phonon coupling is too weak to account for the superconductivity Tc in all three materials. It implies the existence of unconventional pairing of these kagome metals. Our results provide essential knowledge toward understanding the superconductivity and topology in kagome metals.

We report the discovery of a new three-dimensional (3D) topological Dirac semimetal (TDS) material KZnBi, coexisting with a naturally formed superconducting state on the surface under ambient pressure. Using photoemission spectroscopy together with first-principles calculations, a 3D Dirac state with linear band dispersion is identified. The characteristic features of massless Dirac fermions are also confirmed by magnetotransport measurements, exhibiting an extremely small cyclotron mass of m∗=0.012 m0 and a high Fermi velocity of vF=1.04×106 m/s. Interestingly, superconductivity occurs below 0.85 K on the (001) surface, while the bulk remains nonsuperconducting. The captured linear temperature dependence of the upper critical field suggests the possible non-s-wave character of this surface superconductivity. Our discovery serves a distinctive platform to study the interplay between 3D TDS and the superconductivity.

Research on the anomalous Hall effect (AHE) has been lasting for a century to make clear the underlying physical mechanism. Generally, the AHE appears in magnetic materials, in which the extrinsic process related to scattering effects and intrinsic contribution connected with Berry curvature are crucial. Recently, AHE has been counterintuitively observed in nonmagnetic topological materials and attributed to the existence of Weyl points. However, the Weyl point scenario would lead to unsaturated AHE even in large magnetic fields and contradicts the saturation of AHE in several tesla (T) in experiments. In this work, we investigate the Hall effect of ZrTe5 and HfTe5 thin flakes in static ultrahigh magnetic fields up to 33 T. We find the AHE saturates to 55(70)Ω1cm1 for ZrTe5 (HfTe5) thin flakes above ~10T. Combining detailed magnetotransport experiments and Berry curvature calculations, we clarify that the splitting of massive Dirac bands without Weyl points can be responsible for AHE in nonmagnetic topological materials ZrTe5 and HfTe5 thin flakes. This model can identify our thin flake samples to be weak topological insulators and serve as a tool to probe the band structure topology in topological materials.

Discoveries of topological states and topological materials have reshaped our understanding of physics and materials over the past 15 years. First-principles calculations have had an important role in bridging the theory of topology and experiments by predicting realistic topological materials. In this Review, we offer an overview of the first-principles methodology on topological quantum materials. First, we unify different concepts of topological states in the same band inversion scenario. We then discuss the topology using first-principles band structures and newly established topological materials databases. We stress challenges in characterizing symmetry-independent Weyl semimetals and calculating topological surface states, closing with an outlook on the exciting transport and optical phenomena induced by the topology.

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 side 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 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 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 layered antiferromagnetic MnBi2Te4 films have been proposed to be an intrinsic quantum anomalous Hall (QAH) insulator with a large gap. It is crucial to open a magnetic gap of surface states. However, recent experiments have observed gapless surface states, indicating the absence of out-of-plane surface magnetism, and thus, the quantized Hall resistance can only be achieved at the magnetic field above 6 T. We propose to induce out-of-plane surface magnetism of MnBi2Te4 films via the magnetic proximity with magnetic insulator CrI3. A strong exchange bias of similar to 40 meV originates from the long Cr-e(g) orbital tails that hybridize strongly with Te p orbitals. By stabilizing surface magnetism, the QAH effect can be realized in the MnBi2Te4/CrI3 heterostructure. Moreover, the high-Chern number QAH state can be achieved by controlling external electric gates. Thus, the MnBi2Te4/CrI3 heterostructure provides a promising platform to realize the electrically tunable zero-field QAH effect.

In large-scale computations of physical problems, one often encounters the situation of having to determine a multidimensional function, which can be numerically costly when computing each point in this multidimensional space is already time-demanding. In the work, we propose that the active learning algorithm can speed up such calculations. The basic idea is to fit a multidimensional function by neural networks, and the key point is to make the query of labeled data more economical by using a strategy called "query by committee."We present the general protocol of this fitting scheme, as well as the procedure of how to further compute physical observables with the fitted functions. We show that this method can work well with two examples, which are the quantum three-body problem in atomic physics and the anomalous Hall conductivity in condensed matter physics, respectively. In these examples, we show that one reaches an accuracy of a few percent error in computing physical observables, all the while using fewer than 10% of total data points compared with uniform sampling. With these two examples, we also visualize that by using the active learning algorithm, the required amount of data points are added mostly in the regime where the function varies most rapidly, which explains the mechanism for the efficiency of the algorithm. We expect broad applications of our method to various kinds of computational physical problems.

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.

In the version of this Review Article originally published, three of the citations corresponded to the wrong references. Ref. 16 should have corresponded to Nature 533, 513-516 (2016), ref. 17 to Nat. Mater. 16, 94-100 (2016), and ref. 18 to Phys. Rev. Appl. 6, 054001 (2016).

The spin Hall effect (SHE), which converts a charge current into a transverse spin current, has long been believed to be a phenomenon induced by spin-orbit coupling. Here, we identify an alternative mechanism to realize the intrinsic SHE through a noncollinear magnetic structure that breaks the spin rotation symmetry. No spin-orbit coupling is needed even when the scalar spin chirality vanishes, different from the case of the topological Hall effect and topological SHE reported previously. In known noncollinear antiferromagnetic compounds Mn3X (X = Ga, Ge, and Sn), for example, we indeed obtain large spin Hall conductivities based on ab initio calculations.

Using first-principles calculations, we investigate the photogalvanic effect in the Weyl semimetal material TaAs. We find colossal photocurrents caused by the Weyl points in the band structure in a wide range of laser frequency. Our calculations reveal that the photocurrent is predominantly contributed by the three-band transition from the occupied Weyl band to the empty Weyl band via an intermediate band away from the Weyl cone, for excitations both by linearly and circularly polarized light. Therefore, it is essential to sum over all three-band transitions by considering a full set of Bloch bands (both Weyl bands and trivial bands) in the first-principles band structure while it does not suffice to only consider the two-band direct transition within a Weyl cone. The calculated photoconductivities are well consistent with recent experiment measurements. Our work provides a first-principles calculation on nonlinear optical phenomena of Weyl semimetals and provides a deeper understanding of the photogalvanic effects in complexed materials.

Recently, an air-stable layered semiconductor Bi2O2Se was discovered to exhibit an ultrahigh mobility in transistors fabricated with its thin layers. In this work, we explored the mechanism that induces the high mobility and distinguishes Bi2O2Se from other semiconductors. We found that the electron donor states lie above the lowest conduction band. Thus, electrons get spontaneously ionized from donor sites (e.g., Se vacancies) without involving the thermal activation, different from the donor ionization in conventional semiconductors. Consequently, the resistance decreases as reducing the temperature as observed in our measurement, which is similar to a metal but contrasts to a usual semiconductor. Furthermore, the electron conduction channels locate spatially away from ionized donor defects (Se vacancies) in different van der Waals layers. Such a spatial separation can strongly suppress the scattering caused by donor sites and subsequently increase the electron mobility, especially at the low temperature. We call this high-mobility mechanism self-modulation doping, i.e., the modulation doping spontaneously happening in a single-phase material without requiring a heterojunction. Our work paves a way to design high-mobility semiconductors with layered materials.

The recent demonstrations of electrical manipulation and detection of antiferromagnetic spins have opened up a new chapter in the story of spintronics. Here, we review the emerging research field that is exploring the links between antiferromagnetic spintronics and topological structures in real and momentum space. Active topics include proposals to realize Majorana fermions in antiferromagnetic topological superconductors, to control topological protection and Dirac points by manipulating antiferromagnetic order parameters, and to exploit the anomalous and topological Hall effects of zero-net-moment antiferromagnets. We explain the basic concepts behind these proposals, and discuss potential applications of topological antiferromagnetic spintronics.Correction: In the version of this Review Article originally
published, three of the citations corresponded to the wrong references. Ref. 16
should have corresponded to Nature 533, 513516 (2016),
ref. 17 to Nat. Mater. 16, 94100 (2016), and ref. 18
to Phys. Rev. Appl. 6, 054001 (2016).

In addition, in Fig. 1e, the thin black data line should
have been a continuation of the thick blue one; the credit citations for
panels b and c of Fig. 5 were the wrong way
around; they should have been to ref. 96 for b and ref. 93
for c; and references 108, 109 and 110 were appearing out of order,
though correctly cited.

We introduce a class of two-dimensional (2D) materials that possess coexisting ferroelectric and topologically insulating orders. Such ferroelectric topological insulators (FETIs) occur in noncentrosymmetric atomic layer structures with strong spin-orbit coupling (SOC). We showcase a prototype 2D FETI in an atomically thin bismuth layer functionalized by CH2OH, which exhibits a large ferroelectric polarization that is switchable by a ligand molecule rotation mechanism and a strong SOC that drives a band inversion leading to the topologically insulating state. An external electric field that switches the ferroelectric polarization also tunes the spin texture in the underlying atomic lattice. Moreover, the functionalized bismuth layer exhibits an additional quantum order driven by the valley splitting at the K and K' points in the Brillouin zone stemming from the symmetry breaking and strong SOC in the system, resulting in a remarkable state of matter with the simultaneous presence of the quantum spin Hall and quantum valley Hall effect. These phenomena are predicted to exist in other similarly constructed 2D FETIs, thereby offering a unique quantum material platform for discovering novel physics and exploring innovative applications.

Noncollinear antiferromagnets, such as Mn3Sn and Mn3Ir, 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.

The Ta181 quadrupole resonance [nuclear quadrupole resonance (NQR)] technique is utilized to investigate the microscopic magnetic properties of the Weyl semimetal TaP. We find three zero-field NQR signals associated with the transition between the quadrupole split levels for Ta with I=7/2 nuclear spin. A quadrupole coupling constant, νQ=19.250 MHz, and an asymmetric parameter of the electric field gradient, η=0.423, are extracted, in good agreement with band structure calculations. In order to examine the magnetic excitations, the temperature dependence of the spin-lattice relaxation rate (1/T1T) is measured for the f2 line (±5/2↔±3/2 transition). We find that there exist two regimes with quite different relaxation processes. Above T∗≈30 K, a pronounced (1/T1T) T2 behavior is found, which is attributed to the magnetic excitations at the Weyl nodes with temperature-dependent orbital hyperfine coupling. Below T∗, the relaxation is mainly governed by a Korringa process with 1/T1T=const, accompanied by an additional T-1/2-type dependence to fit our experimental data. We show that Ta NQR is a novel probe for the bulk Weyl fermions and their excitations.

High-mobility semiconducting ultrathin films form the basis of modern electronics, and may lead to the scalable fabrication of highly performing devices. Because the ultrathin limit cannot be reached for traditional semiconductors, identifying new two-dimensional materials with both high carrier mobility and a large electronic bandgap is a pivotal goal of fundamental research^1-9. However, air-stable ultrathin semiconducting materials with superior performances remain elusive at present¹⁰. Here, we report ultrathin films of non-encapsulated layered Bi₂O₂ Se, grown by chemical vapour deposition, which demonstrate excellent air stability and high-mobility semiconducting behaviour. We observe bandgap values of ∼0.8 eV, which are strongly dependent on the film thickness due to quantum-confinement effects. An ultrahigh Hall mobility value of >20,000 cm² V^-1 s^-1 is measured in as-grown Bi₂O₂ Se nanoflakes at low temperatures. This value is comparable to what is observed in graphene grown by chemical vapour deposition¹¹ and at the LaAlO₃-SrTiO₃ interface¹², making the detection of Shubnikov-de Haas quantum oscillations possible. Top-gated field-effect transistors based on Bi₂O₂ Se crystals down to the bilayer limit exhibit high Hall mobility values (up to 450 cm² V ^-1 s^-1), large current on/off ratios (>10⁶) and near-ideal subthreshold swing values (∼65 mV dec^-1) at room temperature. Our results make Bi₂O₂ Se a promising candidate for future high-speed and low-power electronic applications.

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 higher the energy of a particle is above equilibrium, the faster it relaxes because of the growing phase space of available electronic states it can interact with. In the relaxation process, phase coherence is lost, thus limiting high-energy quantum control and manipulation. In one-dimensional systems, high relaxation rates are expected to destabilize electronic quasiparticles. Here, we show that the decoherence induced by relaxation of hot electrons in one-dimensional semiconducting nanowires evolves nonmonotonically with energy such that above a certain threshold hot electrons regain stability with increasing energy. We directly observe this phenomenon by visualizing, for the first time, the interference patterns of the quasi-one-dimensional electrons using scanning tunneling microscopy. We visualize the phase coherence length of the one-dimensional electrons, as well as their phase coherence time, captured by crystallographic Fabry-Pèrot resonators. A remarkable agreement with a theoretical model reveals that the nonmonotonic behavior is driven by the unique manner in which one-dimensional hot electrons interact with the cold electrons occupying the Fermi sea. This newly discovered relaxation profile suggests a high-energy regime for operating quantum applications that necessitate extended coherence or long thermalization times, and may stabilize electronic quasiparticles in one dimension.Errata: This paper was published online on 5 May 2017 with
an error in the author list. The eighth authors name should read as \u201cTorsten
Karzig.\u201d The author name has been corrected as of 22 May 2017.

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.

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.

Weyl semimetals are often considered the 3D-analogon of graphene or topological insulators. The evaluation of quantum oscillations in these systems remains challenging because there are often multiple conduction bands. We observe de Haas-van Alphen oscillations with several frequencies in a single crystal of the Weyl semimetal niobium phosphide. For each fundamental crystal axis, we can fit the raw data to a superposition of sinusoidal functions, which enables us to calculate the characteristic parameters of all individual bulk conduction bands using Fourier transform with an analysis of the temperature and magnetic field-dependent oscillation amplitude decay. Our experimental results indicate that the band structure consists of Dirac bands with low cyclotron mass, a non-trivial Berry phase and parabolic bands with a higher effective mass and trivial Berry phase.

Since their discovery, topological insulators are expected to be ideal spintronic materials owing to the spin currents carried by surface states with spin-momentum locking. However, the bulk doping problem remains an obstacle that hinders such an application. In this work, we predict that a newly discovered family of topological materials, the Weyl semimetals, exhibits a large intrinsic spin Hall effect that can be utilized to generate and detect spin currents. Our ab initio calculations reveal a large spin Hall conductivity in the TaAs family of Weyl materials. Considering the low charge conductivity of semimetals, Weyl semimetals are believed to present a larger spin Hall angle (the ratio of the spin Hall conductivity over the charge conductivity) than that of conventional spin Hall systems such as the 4d and 5d transition metals. The spin Hall effect originates intrinsically from the bulk band structure of Weyl semimetals, which exhibit a large Berry curvature and spin-orbit coupling, so the bulk carrier problem in the topological insulators is naturally avoided. Our work not only paves the way for employing Weyl semimetals in spintronics, but also proposes a new guideline for searching for the spin Hall effect in various topological materials.

Quantum spin Hall (QSH) insulates exist in special two-dimensional (2D) semiconductors, possessing the quantized spin-Hall conductance that are topologically protected from backscattering. Based on the first-principles calculations, we predict a novel family of QSH insulators in 2D tantalum carbide halides TaCX (X=Cl, Br, and I) with unique rectangular lattice and large direct energy gaps. The mechanism for 2DQSHeffect originates from an intrinsic d-d band inversion in the process of chemical bonding. Further, stain and intrinsic electric field can be used to tune the electronic structure and enhance the energy gap. TaCX nanoribbon, which has the single-Dirac-cone edge states crossing the bulk band gap, exhibits a linear dispersion with a high Fermi velocity comparable to that of graphene. These 2D materials with considerable nontrivial gaps promise great application potential in the new generation of dissipationless electronics and spintronics.

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%).

We report on the pressure evolution of the Fermi surface topology of the Weyl semimetal NbP, probed by Shubnikov-de Haas oscillations in the magnetoresistance combined with ab initio calculations of the band structure. Although we observe a drastic effect on the amplitudes of the quantum oscillations, the frequencies only exhibit a weak pressure dependence up to 2.8 GPa. The pressure-induced variations in the oscillation frequencies are consistent with our band-structure calculations. Furthermore, we can relate the changes in the amplitudes to small modifications in the shape of the Fermi surface. Our findings show evidence of the stability of the electronic band structure of NbP and demonstrate the power of combining quantum-oscillation studies and band-structure calculations to investigate pressure effects on the Fermi surface topology in Weyl semimetals.

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.

Graphene is the first model system of two-dimensional topological insulator (TI), also known as quantum spin Hall (QSH) insulator. The QSH effect in graphene, however, has eluded direct experimental detection because of its extremely small energy gap due to the weak spin-orbit coupling. Here we predict by ab initio calculations a giant (three orders of magnitude) proximity induced enhancement of the TI energy gap in the graphene layer that is sandwiched between thin slabs of Sb₂Te₃ (or MoTe₂). This gap (1.5 meV) is accessible by existing experimental techniques, and it can be further enhanced by tuning the interlayer distance via compression. We reveal by a tight-binding study that the QSH state in graphene is driven by the Kane-Mele interaction in competition with Kekulé deformation and symmetry breaking. The present work identifies a new family of graphene-based TIs with an observable and controllable bulk energy gap in the graphene layer, thus opening a new avenue for direct verification and exploration of the long-sought QSH effect in graphene.

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 discovered in recent years. They are beyond the spontaneous symmetry-breaking description by Landau and are instead characterized by topological invariants, and described by topological field theory. Their topological nature is similar to the quantum Hall effect, a major discovery of condensed-matter physics in 1980s (Klaus von Klitzing, Nobel Prize in Physics, 1985). The manifestation of the topological effect is the existence of robust gapless surface states inside the bulk energy gap. The topological surface states exhibit Dirac-cone-like energy dispersion with strong spin-momentum locking. Potential future applications cover areas such as spintronics, thermoelectrics, quantum computing and beyond. It is remarkable that TIs have been realized in many common materials, without the requirement of extreme conditions such as high magnetic field and low temperature. The first TI was predicted in 2006 and experimentally realized in 2007 in HgTe quantum wells. Soon afterwards, three traditionally well-known binary chalcogenides, Bi₂Se₃, Bi₂Te₃ and Sb₂Te₃, were predicted and observed to be TIs with a large bulk gap and a metallic surface state consisting of a single Dirac cone. The discovery of these topological materials opened up the exciting field of topological insulators. Extensive experimental and theoretical efforts are devoted to synthesizing and optimizing samples, characterizing the topological states by surface sensitive spectroscopy, transport measurements, device fabrications, and searching for new material candidates. The field of TIs is now expanding at a rapid pace in the communities of physics, chemistry and materials science. In this Focus Issue, we intend to present a high-quality snapshot of the materials and applications aspect of this field. We present ten Review papers from both experiment and theory aspects. Five experimental papers [1-5] overview recent status and challenges of TI nanostructures [1], magnetotransport and induced superconductivity [2], chemistry of Bi-based TI materials [3], molecular beam epitaxial growth of TI thin films [4], and angle-resolved photoemission spectroscopy (ARPES) with circular dichroism [5]. On the other hand, five theoretical papers [6-10] report the progress from different perspectives: materials design by first-principles calculations [6, 7], the relations between TIs and thermoelectric materials [8], Floquet TIs [9], and the classification of topological states [10]. We present ten Letters that cover various aspects, ranging from ARPES, transport measurement and devices, thin film growth to first-principles simulations and fundamental theory. Letters on ARPES [11-14] report the surface states of HgTe [11], Bi₂Se₃ [12, 13] and Bi₂Te₃ [11, 14], in which the surface modification, defect doping and electron-phonon coupling are discussed; a paper on transport experiments [15] demonstrates the coexistence of electron- and hole-type charge carriers in devices of Sb₂Te₃/Bi₂Te₃ heterostructures; the growth of YPtSb thin film is reported [16], which is a Heusler compound near the boundary of topological trivial-nontrivial transition. Corresponding to the ARPES experiments, a Letter of band structure calculations [17] also reveals the effect of vacancy defects on Bi₂Se₃ surface states; another paper [18] shows the dependence of edge state dispersion on edge geometry of graphene. Last but not the least, two papers on phenomenological models [19, 20] report the maximally localized flat-band Hamiltonians and the spectra flow for Aharonov-Bohm rings, respectively. We hope that this Focus Issue will be helpful for your research and stimulate more activity in the exciting field of topological insulators.

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.

We propose new topological insulators in cerium-filled skutterudite (FS) compounds based on ab initio calculations. We find that two compounds, CeOs ₄As ₁₂ and CeOs ₄Sb ₁₂, are zero gap materials with band inversions between Os-d and Ce-f orbitals, similar to HgTe. Both compounds are predicted to become topological Kondo insulators at low temperatures, which are Kondo insulators in the bulk but with robust Dirac surface states on the boundary. Furthermore, this family of topological insulators has more unique features. Due to similar lattice parameters there will be a good proximity effect with other superconducting FS compounds, which may realize Majorana fermions. Additionally, the experimentally observed antiferromagnetic phase of CeOs ₄Sb ₁₂ at very low temperature provides a way to realize the massive Dirac fermion with topological magnetoelectric effects.

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.