Spin-triplet superconductivity from excitonic effect in doped insulators.

SignificanceWe present a mechanism for unconventional superconductivity in doped band insulators, where short-ranged pairing interaction arises from Coulomb repulsion due to virtual interband or excitonic processes. Remarkably, electron pairing is found upon infinitesimal doping, giving rise to Bose-Einstein condensate (BEC)-Bardeen-Cooper-Schrieffer (BCS) crossover at low density. Our theory explains puzzling behaviors of superconductivity and predicts spin-triplet pairing in electron-doped ZrNCl and WTe2.

Negative Differential Resistance with Ultralow Peak-to-Valley Voltage Difference in Td-WTe2/2H-MoS2 Heterostructure.

Negative differential resistance (NDR) devices with a low peak-to-valley voltage difference (ΔV) exhibit a high cut off frequency and low power consumption efficiency, which is significant for fabricating high-performance oscillators. However, achieving an ultralow ΔV is challenging. In this work, we report the first construction of an NDR device utilizing a van der Waals heterostructure composed of semimetallic Td-WTe2 and semiconducting 2H-MoS2. Our findings reveal that the narrow energy region of the decreasing density of states (DOS) above the Fermi level of WTe2 acts as a narrow band gap, facilitating type-III band alignment with MoS2 and enabling band-to-band tunneling-based NDR transport. Notably, the NDR device exhibits an ultralow ΔV of approximately 0.01 V, which is at least an order of magnitude lower than previously reported values. This work not only introduces a new approach for NDR device fabrication but also provides new insights into the pivotal role of Td-WTe2 in NDR transport.

Bias-dependent photoresponse of Td-WTe2grown by chemical vapor deposition.

The type-II Weyl semimetal Td-WTe2is one of the wonder materials for high-performance optoelectronic devices. We report the self-powered Td-WTe2photodetectors and their bias-dependent photoresponse in the visible region (405, 520, 638 nm) driven by the bulk photovoltaic effect. The device shows the responsivity of 15.8 mAW-1and detectivity of 5.2 × 109Jones at 520 nm. Besides, the response time of the WTe2photodetector shows the strong bias-voltage dependent property. This work offers a physical reference for understanding the photoresponse process of Td-WTe2photodetectors.

Atomic Resolution Imaging of Highly Air-Sensitive Monolayer and Twisted-Bilayer WTe2.

Bulk Td-WTe2 is a semimetal, while its monolayer counterpart is a two-dimensional (2D) topological insulator. Recently, electronic transport resembling a Luttinger liquid state was found in twisted-bilayer WTe2 (tWTe2) with a twist angle of ∼5°. Despite the strong interest in 2D WTe2 systems, little experimental information is available about their intrinsic microstructure, leaving obstacles in modeling their physical properties. The monolayer, and consequently tWTe2, are highly air-sensitive, and therefore, probing their atomic structures is difficult. In this study, we develop a robust method for atomic-resolution visualization of monolayers and tWTe2 obtained through mechanical exfoliation and fabrication. We confirm the high crystalline quality of mechanically exfoliated WTe2 samples and observe that tWTe2 with twist angles of ∼5 and ∼2° retains its pristine moiré structure without substantial deformations or reconstructions. The results provide a structural foundation for future electronic modeling of monolayer and tWTe2 moiré lattices.

Symmetry Engineering in Twisted Bilayer WTe2.

The fabrication of artificial structures using a twisted van der Waals assembly has been a key technique for recent advancements in the research of two-dimensional (2D) materials. To date, various exotic phenomena have been observed thanks to the modified electron correlation or moiré structure controlled by the twist angle. However, the twisted van der Waals assembly has further potential to modulate the physical properties by controlling the symmetry. In this study, we fabricated twisted bilayer WTe2 and demonstrated that the twist angle successfully controls the spatial inversion symmetry and hence the spin splitting in the band structure. Our results reveal the further potential of a twisted van der Waals assembly, suggesting the feasibility of pursuing new physical phenomena in 2D materials based on the control of symmetry.

Current-Phase Relation of a WTe2 Josephson Junction.

When a topological insulator is incorporated into a Josephson junction, the system is predicted to reveal the fractional Josephson effect with a 4π-periodic current-phase relation. Here, we report the measurement of a 4π-periodic switching current through an asymmetric SQUID, formed by the higher-order topological insulator WTe2. Contrary to the established opinion, we show that a high asymmetry in critical current and negligible loop inductance are not sufficient by themselves to reliably measure the current-phase relation. Instead, we find that our measurement is heavily influenced by additional inductances originating from the self-formed PdTex inside the junction. We therefore develop a method to numerically recover the current-phase relation of the system and find the 1.5 µm long junction to be best described in the short ballistic limit. Our results highlight the complexity of subtle inductance effects that can give rise to misleading topological signatures in transport measurements.

Pseudo-Hydrodynamic Flow of Quasiparticles in Semimetal WTe2 at Room Temperature.

Recently, much interest has emerged in fluid-like electric charge transport in various solid-state systems. The hydrodynamic behavior of the electronic fluid reveals itself as a decrease of the electrical resistance with increasing temperature (the Gurzhi effect) in narrow channels, polynomial scaling of the resistance as a function of the channel width, violation of the Wiedemann-Franz law supported by the emergence of the Poiseuille flow. Similar to whirlpools in flowing water, the viscous electronic flow generates vortices, resulting in abnormal sign-changing electrical response driven by backflow. However, the question of whether the long-ranged sign-changing electrical response can be produced by a mechanism other than hydrodynamics has not been addressed so far. Here polarization-sensitive laser microscopy is used to demonstrate the emergence of visually similar abnormal sign-alternating patterns in semi-metallic tungsten ditelluride at room temperature where this material does not exhibit true hydrodynamics. It is found that the neutral quasiparticle current consisting of electrons and holes obeys an equation remarkably similar to the Navier-Stokes equation. In particular, the momentum relaxation is replaced by the much slower process of quasiparticle recombination. This pseudo-hydrodynamic flow of quasiparticles leads to a sign-changing charge accumulation pattern via different diffusivities of electrons and holes.

Hybrid mixed-dimensional WTe2/CsPbI3perovskite heterojunction for high-performance photodetectors.

Perovskites have showed significant potential for the application in photodetectors due to their outstanding electrical and optical properties. Integrating two-dimensional (2D) materials with perovskites can make full use of the high carrier mobility of 2D materials and strong light absorption of perovskite to realize excellent optoelectrical properties. Here, we demonstrate a photodetector based on the WTe2/CsPbI3heterostructure. The quenching and the shortened lifetime of photoluminescence (PL) for CsPbI3perovskite confirms the efficient charge transfer at the WTe2/CsPbI3heterojunction. After coupled with WTe2, the photoresponsivity of the CsPbI3photodetector is improved by almost two orders of magnitude due to the high-gain photogating effect. The WTe2/CsPbI3heterojunction photodetector reveals a large responsivity of 1157 A W-1and a high detectivity of 2.1 × 1013Jones. The results pave the way for the development of high-performance optoelectronic devices based on 2D materials/perovskite heterojunctions.

Boosting Electrocatalytic Reduction of CO2 to HCOOH on Ni Single Atom Anchored WTe2 Monolayer.

Achieving efficient conversion of carbon dioxide (CO2 ) to formic acid (HCOOH) at mild conditions is a promising means to reduce greenhouse gas emission and mitigate the energy crisis. Herein, spin-polarized density functional theory calculations with van der Waals corrections (DFT+D3) are performed to analyze the catalytic activity of seven metals (Ti, Fe, Ni, Cu, Zn, In, and Sn) anchored on a tungsten ditelluride monolayer (M@WTe2 ) and screen favorable CO2 reduction pathways. These results demonstrate that Ni single atoms strongly bind to the WTe2 monolayer and exist in isolated form due to the high diffusion barriers. Also, Ni-anchored WTe2 monolayer (Ni@WTe2 ) possesses a considerably low limiting-potential (-0.11 V vs reversible hydrogen electrode) to convert CO2 to HCOOH due to moderate OCHO adsorption energy and a suppressed competing hydrogen evolution reaction (HER). Therefore, Ni@WTe2 monolayer is a promising electrocatalytic material for the CO2 reduction reaction (CO2 RR). This study sheds light on strategies of designing single metal atom anchored WTe2 catalysts for improved CO2 RR performances.

Water-assisted controllable growth of atomically thin WTe2nanoflakes by chemical vapor deposition based on precursor design and substrate engineering strategies.

WTe2nanostructures have intrigued much attention due to their unique properties, such as large non-saturating magnetoresistance, quantum spin Hall effect and topological surface state. However, the controllable growth of large-area atomically thin WTe2nanostructures remains a significant challenge. In the present work, we demonstrate the controllable synthesis of 1T' atomically thin WTe2nanoflakes (NFs) by water-assisted ambient pressure chemical vapor deposition method based on precursor design and substrate engineering strategies. The introduction of water during the growth process can generate a new synthesized route by reacting with WO3to form intermediate volatile metal oxyhydroxide. Using WO3foil as the growth precursor can drastically enhance the uniformity of as-prepared large-area 1T' WTe2NFs compared to WO3powders. Moreover, highly oriented WTe2NFs with distinct orientations can be obtained by using a-plane and c-plane sapphire substrates, respectively. Corresponding precursor design and substrate engineering strategies are expected to be applicable to other low dimensional transition metal dichalcogenides, which are crucial for the design of novel electronic and optoelectronic devices.

Magnetoelastoresistance in WTe2: Exploring electronic structure and extremely large magnetoresistance under strain.

Strain describes the deformation of a material as a result of applied stress. It has been widely employed to probe transport properties of materials, ranging from semiconductors to correlated materials. In order to understand, and eventually control, transport behavior under strain, it is important to quantify the effects of strain on the electronic bandstructure, carrier density, and mobility. Here, we demonstrate that much information can be obtained by exploring magnetoelastoresistance (MER), which refers to magnetic field-driven changes of the elastoresistance. We use this powerful approach to study the combined effect of strain and magnetic fields on the semimetallic transition metal dichalcogenide [Formula: see text] We discover that WTe2 shows a large and temperature-nonmonotonic elastoresistance, driven by uniaxial stress, that can be tuned by magnetic field. Using first-principle and analytical low-energy model calculations, we provide a semiquantitative understanding of our experimental observations. We show that in [Formula: see text], the strain-induced change of the carrier density dominates the observed elastoresistance. In addition, the change of the mobilities can be directly accessed by using MER. Our analysis also reveals the importance of a heavy-hole band near the Fermi level on the elastoresistance at intermediate temperatures. Systematic understanding of strain effects in single crystals of correlated materials is important for future applications, such as strain tuning of bulk phases and fabrication of devices controlled by strain.

Spin-Momentum Locking Induced Anisotropic Magnetoresistance in Monolayer WTe2.

Monolayer WTe2 is predicted to be a quantum spin Hall insulator (QSHI), and its quantized edge transport has recently been demonstrated. However, one of the essential properties of a QSHI, spin-momentum locking of the helical edge states, has yet to be experimentally validated. Here, we measure and observe gate-controlled anisotropic magnetoresistance (AMR) in monolayer WTe2 devices. Electrically tuning the Fermi energy into the band gap, a large in-plane AMR is observed and the minimum of the in-plane AMR occurs when the applied magnetic field is perpendicular to the current direction. In line with the experimental observations, the theoretical predictions based on the band structure of monolayer WTe2 demonstrate that the AMR effect originates from spin-momentum locking in the helical edge states of monolayer WTe2. Our findings reveal that the spin quantization axis of the helical edge states in monolayer WTe2 can be precisely determined from AMR measurements.

Weyl semimetal orthorhombic Td-WTe2as an electrode material for sodium- and potassium-ion batteries.

Alkali metals such as sodium and potassium have become promising candidates for the next generation of monovalent-ion batteries. However, a challenge for these battery technologies lies in the development of electrode materials that deliver high capacity and stable performance even at high cycling currents. Here we study orthorhombic tungsten ditelluride or Td-WTe2as an electrode material for sodium- (SIB) and potassium-ion batteries (KIB) in propylene carbonate (PC) based electrolyte. Results show that despite larger Shannon's radius of potassium-ions and their sluggish diffusion in Td-WTe2due to higher overpotential, at 100 mA.g-1KIB-half cells showed higher cycling stability and low capacity decay of 4% versus 16% compared to SIB-half cells. Likewise, in a rate capability test at 61stcycle (at 50 mA.g-1), the KIB-half cells yielded charge capacity of 172 mAh.g-1versus 137 mAh.g-1of SIB-half cells. The superior electrochemical performance of Td-WTe2electrode material in KIB-half cells is explained based on the concept of Stokes' radius-smaller desolvation activation energy resulted in higher mobility of potassium-ions in PC-based electrolyte. In addition, the likely mechanisms of electrochemical insertion and extraction of Na- and K-ions in Td-WTe2are also discussed.

One-Dimensional Edge Transport in Few-Layer WTe2.

WTe2 is a layered transitional-metal dichalcogenide (TMD) with a number of intriguing topological properties. Recently, WTe2 has been predicted to be a higher-order topological insulator (HOTI) with topologically protected hinge states along the edges. The gapless nature of WTe2 complicates the observation of one-dimensional (1D) topological states in transport due to their small contribution relative to the bulk. Here, we study the behavior of the Josephson effect in magnetic field to distinguish edge from bulk transport. The Josephson effect in few-layer WTe2 reveals 1D states residing on the edges and steps. Moreover, our data demonstrates a combination of Josephson transport properties observed solely in another HOTI-bismuth, including Josephson transport over micrometer distances, extreme robustness in a magnetic field, and nonsinusoidal current-phase relation (CPR). Our observations strongly suggest the topological origin of the 1D states and that few-layer WTe2 is a HOTI.

Microfocus Laser-Angle-Resolved Photoemission on Encapsulated Mono-, Bi-, and Few-Layer 1T'-WTe2.

Two-dimensional crystals of semi-metallic van der Waals materials hold much potential for the realization of novel phases, as exemplified by the recent discoveries of a polar metal in few-layer 1T'-WTe2 and of a quantum spin Hall state in monolayers of the same material. Understanding these phases is particularly challenging because little is known from experiments about the momentum space electronic structure of ultrathin crystals. Here, we report direct electronic structure measurements of exfoliated mono-, bi-, and few-layer 1T'-WTe2 by laser-based microfocus angle-resolved photoemission. This is achieved by encapsulating with monolayer graphene a flake of WTe2 comprising regions of different thickness. Our data support the recent identification of a quantum spin Hall state in monolayer 1T'-WTe2 and reveal strong signatures of the broken inversion symmetry in the bilayer. We finally discuss the sensitivity of encapsulated samples to contaminants following exposure to ambient atmosphere.

Anomalous Photothermoelectric Transport Due to Anisotropic Energy Dispersion in WTe2.

Band structures are vital in determining the electronic properties of materials. Recently, the two-dimensional (2D) semimetallic transition metal tellurides (WTe2 and MoTe2) have sparked broad research interest because of their elliptical or open Fermi surface, making distinct from the conventional 2D materials. In this study, we demonstrate a centrosymmetric photothermoelectric voltage distribution in WTe2 nanoflakes, which has not been observed in common 2D materials such as graphene and MoS2. Our theoretical model shows the anomalous photothermoelectric effect arises from an anisotropic energy dispersion and micrometer-scale hot carrier diffusion length of WTe2. Further, our results are more consistent with the anisotropic tilt direction of energy dispersion being aligned to the b-axis rather than the a-axis of the WTe2 crystal, which is consistent with the previous first-principle calculations as well as magneto-transport experiments. Our work shows the photothermoelectric current is strongly confined to the anisotropic direction of the energy dispersion in WTe2, which opens an avenue for interesting electro-optic applications such as electron beam collimation and electron lenses.

Unveiling the Interfacial Effects for Enhanced Hydrogen Evolution Reaction on MoS2 /WTe2 Hybrid Structures.

Using the MoS2 -WTe2 heterostructure as a model system combined with electrochemical microreactors and density function theory calculations, it is shown that heterostructured contacts enhance the hydrogen evolution reaction (HER) activity of monolayer MoS2 . Two possible mechanisms are suggested to explain this enhancement: efficient charge injection through large-area heterojunctions between MoS2 and WTe2 and effective screening of mirror charges due to the semimetallic nature of WTe2 . The dielectric screening effect is proven minor, probed by measuring the HER activity of monolayer MoS2 on various support substrates with dielectric constants ranging from 4 to 300. Thus, the enhanced HER is attributed to the increased charge injection into MoS2 through large-area heterojunctions. Based on this understanding, a MoS2 /WTe2 hybrid catalyst is fabricated with an HER overpotential of -140 mV at 10 mA cm-2 , a Tafel slope of 40 mV dec-1 , and long stability. These results demonstrate the importance of interfacial design in transition metal dichalcogenide HER catalysts. The microreactor platform presents an unambiguous approach to probe interfacial effects in various electrocatalytic reactions.

Proximity-Induced Superconductivity with Subgap Anomaly in Type II Weyl Semi-Metal WTe2.

Due to the nontrivial topological band structure in type II Weyl semi-metal tungsten ditelluride (WTe2), unconventional properties may emerge in its superconducting phase. While realizing intrinsic superconductivity has been challenging in the type II Weyl semi-metal WTe2, the proximity effect may open an avenue for the realization of superconductivity. Here, we report the observation of proximity-induced superconductivity with a long coherence length along the c axis in WTe2 thin flakes based on a WTe2/NbSe2 van der Waals heterostructure. Interestingly, we also observe anomalous oscillations of the differential resistance during the transition from the superconducting to the normal state. Theoretical calculations show excellent agreement with experimental results, revealing that such a subgap anomaly is the intrinsic property of WTe2 in superconducting state induced by the proximity effect. Our findings enrich the understanding of the superconducting phase of type II Weyl semi-metals and pave the way for their future applications in topological quantum computing.

Superconductivity in Potassium-Intercalated T d-WTe2.

To realize a topological superconductor is one of the most attracting topics because of its great potential in quantum computation. In this study, we successfully intercalate potassium (K) into the van der Waals gap of type II Weyl semimetal WTe2 and discover the superconducting state in K xWTe2 through both electrical transport and scanning tunneling spectroscopy measurements. The superconductivity exhibits an evident anisotropic behavior. Moreover, we also uncover the coexistence of superconductivity and the positive magnetoresistance state. Structural analysis substantiates the negligible lattice expansion induced by the intercalation, therefore suggesting K-intercalated WTe2 still hosts the topological nontrivial state. These results indicate that the K-intercalated WTe2 may be a promising candidate to explore the topological superconductor.

Thermopower and Unconventional Nernst Effect in the Predicted Type-II Weyl Semimetal WTe2.

WTe2 is one of a series of recently discovered high mobility semimetals, some of whose properties are characteristic of topological Dirac or Weyl metals. One of its most interesting properties is the unsaturated giant magnetoresistance that it exhibits at low temperatures. An important question is the degree to which this property can be ascribed to a conventional semimetallic model in which a highly compensated, high mobility metal exhibits large magnetoresistance. Here, we show that the longitudinal thermopower (Seebeck effect) of semimetallic WTe2 exfoliated flakes exhibits periodic sign changes about zero with increasing magnetic field that indicates distinct electron and hole Landau levels and nearly fully compensated electron and hole carrier densities. However, inconsistent with a conventional semimetallic picture, we find a rapid enhancement of the Nernst effect at low temperatures that is nonlinear in magnetic field, which is consistent with Weyl points in proximity to the Fermi energy. Hence, we demonstrate the role played by the Weyl character of WTe2 in its transport properties.