Recently, it has been pointed out that the twisting of bilayer WSe$_2$ would generate topologically non-trivial flat bands near the Fermi energy. In this work, we show that twisted bilayer WSe$_2$ (tWSe$_2$) with uniaxial strain exhibits a large nonlinear Hall (NLH) response due to the non-trivial Berry curvatures of the flat bands. Moreover, the NLH effect is greatly enhanced near the topological phase transition point which can be tuned by a vertical displacement field. Importantly, the nonlinear Hall signal changes sign across the topological phase transition point and provides a way to identify the topological phase transition and probe the topological properties of the flat bands. The strong enhancement and high tunability of the NLH effect near the topological phase transition point renders tWSe$_2$ and related moire materials new platforms for rectification and second harmonic generations.
Heterostructures formed between two different van der Waals materials enable interactions and functionalities absent in each component. In this work we show that vicinity to an atomically thin WSe$_2$ sheet dramatically impacts the energies of the symmetry-broken low Landau levels of bilayer graphene, possibly due to screening. We present a systematic study of the magnetic field and electrical displacement field dependences of the Landau level gaps at filling factor $ν$ = 1, 2, 3, and compare to BN encapsulated pristine bilayer graphene. The exchange-dominated energy splitting between the N = …
Proximity orbital and spin-orbit effects of bilayer graphene on monolayer WSe$_2$ are investigated from first-principles. We find that the built-in electric field induces an orbital band gap of about 10 meV in bilayer graphene. Remarkably, the proximity spin-orbit splitting for holes is two orders of magnitude---the spin-orbit splitting of the valence band at K is about 2 meV---more than for electrons. Effectively, holes experience spin-valley locking due to the strong proximity of the lower graphene layer to WSe$_2$. However, applying an external transverse electric field of some 1 V/nm, coun…
Twisted bilayer graphene provides a new two-dimensional platform for studying electron interaction phenomena and flat band properties such as correlated insulator transition, superconductivity and ferromagnetism at certain magic angles. Here, we present strong evidence of correlated insulator states and superconductivity signatures in p-type twisted double-bilayer WSe$_2$. Enhanced interlayer interactions are observed when the twist angle decreases to a few degrees as reflected by the high-order satellites in the electron diffraction patterns taken from the 2H/3R-stacked domains reconstructed …
We show that topology of the low-energy band structure in bilayer graphene critically depends on mechanical deformations of the crystal which may easily develop in suspended graphene flakes. We describe the Lifshitz transition that takes place in strained bilayers upon splitting the parabollic bands at intermediate energies into several Dirac cones at the energy scale of few meV. Then, we show how this affects the electron Landau level spectra and the quantum Hall effect.
We report the experimental observation of strongly enhanced tunneling between graphene bilayers through a WSe$_2$ barrier when the graphene bilayers are populated with carriers of opposite polarity and equal density. The enhanced tunneling increases sharply in strength with decreasing temperature, and the tunneling current exhibits a vertical onset as a function of interlayer voltage at a temperature of 1.5 K. The strongly enhanced tunneling at overall neutrality departs markedly from single-particle model calculations that otherwise match the measured tunneling current-voltage characteristics…
Twist bilayer graphenes with magical angle have nearly flat band, which become strongly correlated electron systems. Herein, we propose another system based on strained bilayer graphene that have flat band at the intrinsic Fermi level. The top and bottom layers are uniaxially stretched along different directions. When the strength and directions of the strain satisfy certain condition, the periodical lattices of the two layers are commensurate to each other. The regions with AA, AB and BA stacking arrange in a triangular lattice. With magical strain, the bands around the intrinsic Fermi level …
We report the direct observation of intervalley exciton between the Q conduction valley and $Γ$ valence valley in bilayer WSe$_2$ by photoluminescence. The Q$Γ$ exciton lies at ~18 meV below the QK exciton and dominates the luminescence of bilayer WSe$_2$. By measuring the exciton spectra at gate-tunable electric field, we reveal different interlayer electric dipole moments and Stark shifts between Q$Γ$ and QK excitons. Notably, we can use the electric field to switch the energy order and dominant luminescence between Q$Γ$ and QK excitons. Both Q$Γ$ and QK excitons exhibit pronounced phonon re…
The large surface-to-volume ratio in atomically thin 2D materials allows to efficiently tune their properties through modifications of their environment. Artificial stacking of two monolayers into a bilayer leads to an overlap of layer-localized wave functions giving rise to a twist angle-dependent hybridization of excitonic states. In this joint theory-experiment study, we demonstrate the impact of interlayer hybridization on bright and momentum-dark excitons in twisted WSe$_2$ bilayers. In particular, we show that the strong hybridization of electrons at the $Λ$ point leads to a drastic reds…
Stacking-order-dependent electronic properties of MoTe2/WSe2 moiré bilayers
Cornell University（康奈尔大学）；Max Planck Institute for the Structure and Dynamics of Matter（马克斯·普朗克物质结构动力学研究所）；Kavli Institute at Cornell for Nanoscale Science（康奈尔纳米科学卡弗里研究所）；National Institute for Materials Science（国立材料研究所）
Lattice reconstruction in twisted transition-metal dichalcogenide (TMD) bilayers gives rise to piezo- and ferroelectric moiré potentials for electrons and holes, as well as a modulation of the hybridisation across the bilayer. Here, we develop hybrid $\mathbf{k}\cdot \mathbf{p}$ tight-binding models to describe electrons and holes in the relevant valleys of twisted TMD homobilayers with parallel (P) and anti-parallel (AP) orientations of the monolayer unit cells. We apply these models to describe moiré superlattice effects in twisted WSe${}_2$ bilayers, in conjunction with microscopic \emph{ab…
Monolayer (ML) transition metal dichalcogenides (TMDs) undergo substantial changes in the single-particle band structure and excitonic optical response upon the addition of just one layer. As opposed to the single-layer limit, the bandgap of bilayer (BL) TMD semiconductors is indirect which results in reduced photoluminescence with richly structured spectra that have eluded a detailed understanding to date. Here, we provide a closed interpretation of the elementary optical responses of BL WSe$_2$ as a representative material for the wider class of TMD semiconductors. By combining theoretical c…
With the both spin and valley degrees of freedom, the low-lying excitonic spectra of photo-excited transition-metal dichalcogenide monolayers (TMDC-MLs) are featured by rich fine structures, comprising the intra-valley bright exciton states as well as various intra- and inter-valley dark ones. The latter states can be classified as those of the spin- and momentum-forbidden dark excitons according to the violated optical selection rules. Because of the optical invisibility, the two types of the dark states are in general hardly observed and even distinguished in conventional spectroscopies alth…
Hybridisation of electronic bands of two-dimensional materials, assembled into twistronic heterostructures, enables one to tune their optoelectronic properties by selecting conditions for resonant interlayer hybridisation. Resonant interlayer hybridisation qualitatively modifies the excitons in such heterostructures, transforming these optically active modes into superposition states of interlayer and intralayer excitons. For MoSe$_2$/WSe$_2$ heterostructures, strong hybridization occurs between the holes in the spin-split valence band of WSe$_2$ and in the top valence band of MoSe$_2$, especi…
We investigate the hole spin relaxation due to the Rashba spin-orbit coupling induced by an external perpendicular electric field in bilayer WSe$_2$. The Rashba spin-orbit coupling coefficients in bilayer WSe$_2$ are constructed from the corresponding monolayer ones. In contrast to monolayer WSe$_2$, the out-of-plane component of the bilayer Rashba spin-orbit coupling acts as a Zeeman-like field with opposite directions but identical values in the two valleys. For in-plane spins, this Zeeman-like field, together with the intervalley hole-phonon scattering, opens an intervalley spin relaxation …
We study the magnetotransport properties of high mobility holes in monolayer and bilayer WSe$_2$, which display well defined Shubnikov-de Haas (SdH) oscillations, and quantum Hall states (QHSs) in high magnetic fields. In both mono and bilayer WSe$_2$, the SdH oscillations and the QHSs occur predominantly at even filling factors, evincing a two-fold Landau level degeneracy. The Fourier transform analysis of the SdH oscillations in bilayer WSe$_2$ reveal the presence of two subbands localized in the top or the bottom layer, as well as negative compressibility. From the temperature dependence of…
Electrode-tunable nonlocal charge to spin conversion in WSe$_2$-intercalated bilayer graphene
Institute of Informatics, Slovak Academy of Sciences（斯洛伐克科学院信息学研究所）；Faculty of Physics, University of Belgrade（贝尔格莱德大学物理学院）；Institute of Physics, Pavol Jozef Šafárik University in Košice（科希策帕维尔·约瑟夫·沙法里克大学物理研究所）；Institute of Experimental Physics, Slovak Academy of Sciences（斯洛伐克科学院实验物理研究所）；New Technologies Research Centre, University of West Bohemia（西波希米亚大学新技术研究中心）
Moiré superlattices in van der Waals heterostructures provide a tunable platform to study emergent properties that are absent in the natural crystal form. Twisted bilayer transition metal dichalcogenides (TB-TMDs) can host moiré flat bands over a wide range of twist angles. For twist angle close to 60°, it was predicted that TB-TMDs undergo a lattice reconstruction which causes the formation of ultra-flat bands. Here, by using scanning tunneling microscopy and spectroscopy, we show the emergence of multiple ultra-flat bands in twisted bilayer WSe2 when the twist angle is larger than 57°. The b…
A valley-contrasting Berry curvature in bilayer transition metal dichalcogenides with spin-orbit coupling can generate valley magnetization when the inversion symmetry is broken, for example, by an electric field, regardless of time-reversal symmetry. A nontrivial Berry curvature can also lead to anomalous transport responses, such as the anomalous Hall effect and the anomalous Nernst effect. Applied to a bilayer WSe$_2$, an electric field can tune the Berry curvature and orbital magnetic moment, which has important consequences for the orbital magnetization and the anomalous Nernst responses.…
Twistronic van der Waals heterostrutures offer exciting opportunities for engineering optoelectronic properties of nanomaterials. Here, we use multiscale modeling to study trapping of charge carriers and excitons by ferroelectric polarisation and piezoelectric charges by domain structures in twistronic WX$_2$/MoX$_2$ bilayers (X=S,Se). For almost aligned 2H-type bilayers, we find that holes and electrons are trapped in the opposite -- WMo and XX (tungsten over molybdenum {\it versus} overlaying chalcogens) -- corners of the honeycomb domain wall network, swapping their position at a twist angl…
We report the fabrication and characterization of gate-defined hole quantum dots in monolayer and bilayer WSe$_2$. The devices were operated with gates above and below the WSe$_2$ layer to accumulate a hole gas, which for some devices was then selectively depleted to define the dot. Temperature dependence of conductance in the Coulomb blockade regime is consistent with transport through a single level, and excited state transport through the dots was observed at temperatures up to 10 K. For adjacent charge states of a bilayer WSe$_2$ dot, magnetic field dependence of excited state energies was…
Recent experiments have measured local uniaxial strain fields in twisted bilayer graphene (TBG). Our calculations found that the finite Berry curvature generated by breaking the sublattice symmetry and the band proximity between narrow bands in these TBG induces a giant Berry dipole of order 10\,nm or larger. The large Berry dipole leads to transverse topological non-linear charge currents which dominates over the linear bulk valley current at experimentally accessible crossover in-plane electric field of $\sim 0.1 {\rm mV} / μ\rm{m}$. This anomalous Hall effect, due to Berry dipole, is strong…
Exciton condensates (EC) are macroscopic coherent states arising from condensation of electron-hole pairs. Bilayer heterostructures, consisting of two-dimensional electron and hole layers separated by a tunnel barrier, provide a versatile platform to realize and study EC. The tunnel barrier suppresses recombination yielding long-lived excitons. However, this separation also reduces interlayer Coulomb interactions, limiting the exciton binding strength. Here, we report the observation of EC in naturally occurring 2H-stacked bilayer WSe$_2$. In this system, the intrinsic spin-valley structure su…
The structural and electronic properties of graphene leads its charge carriers to behave like relativistic particles, which is described by a Dirac-like Hamiltonian. Since graphene is a monolayer of carbon atoms, the strain due to elastic deformations will give rise to so-called `pseudomagnetic fields (PMF)' in graphene sheet, and that has been realized experimentally in strained graphene sample. Here we propose a realistic strained graphene bilayer (SGB) device to detect the pseudo-magnetoexcitons (PME) in the absence of external magnetic field. The carriers in each graphene layer suffer diff…
The optical properties of monolayer and bilayer transition metal dichalcogenide semiconductors are governed by excitons in different spin and valley configurations, providing versatile aspects for van der Waals heterostructures and devices. We present experimental and theoretical studies of exciton energy splittings in external magnetic field in neutral and charged WSe$_2$ monolayer and bilayer crystals embedded in a field effect device for active doping control. We develop theoretical methods to calculate the exciton $g$-factors from first principles and tight-binding for all possible spin-va…
We study the electronic properties of commensurate faulted bilayer graphene by diagonalizing the one-particle Hamiltonian of the bilayer system in a complete basis of Bloch states of the individual graphene layers. Our novel approach is very general and can be easily extended to any commensurate graphene-based heterostructure. Here, we consider three cases: i) twisted bilayer graphene, ii) bilayer graphene where triaxial stress is applied to one layer, and iii) bilayer graphene where uniaxial stress is applied to one layer. We show that the resulting superstructures can be divided into distinc…
The spin Hall effect (SHE), in which electrical current generates transverse spin current, plays an important role in spintronics for the generation and manipulation of spin-polarized electrons. The phenomenon originates from spin-orbit coupling. In general, stronger spin-orbit coupling favors larger SHEs but shorter spin relaxation times and diffusion lengths. To achieve both large SHEs and long-range spin transport in a single material has remained a challenge. Here we demonstrate a giant intrinsic SHE in AB-stacked MoTe2/WSe2 moiré bilayers by direct magneto optical imaging. Under moderate …
Spin-valley 0.7 anomaly in bilayer graphene/WSe$_2$ quantum point contacts
Solid State Physics Laboratory, ETH Zürich（苏黎世联邦理工学院固态物理实验室）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（国立材料研究所材料纳米结构研究中心）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（国立材料研究所电子与光学材料研究中心）；Department of Physics, Ben-Gurion University of the Negev（内盖夫本-古里安大学物理系）
Motivated by a recent experiment [arXiv:2205.05087], we investigate a possible mechanism that enhances superconductivity in hole-doped Bernal bilayer graphene due to a proximate WSe$_2$ monolayer. We show that the virtual tunneling between WSe$_2$ and Bernal bilayer graphene, which is known to induce Ising spin-orbit coupling, can generate an additional attraction between two holes, providing a potential explanation for enhancing superconductivity in Bernal bilayer graphene. Using microscopic interlayer tunneling, we derive the Ising spin-orbit coupling and the effective attraction as function…
Strong gate control of proximity-induced spin-orbit coupling was recently predicted in bilayer graphene/transition metal dichalcogenides (BLG/TMDC) heterostructures, as charge carriers can easily be shifted between the two graphene layers, and only one of them is in close contact to the TMDC. The presence of spin-orbit coupling can be probed by weak antilocalization (WAL) in low field magnetotransport measurements. When the spin-orbit splitting in such a heterostructure increases with the out of plane electric displacement field $\bar D$, one intuitively expects a concomitant increase of WAL v…
Moiré structures in van der Waals heterostructures lead to emergent phenomena including superconductivity in twisted bilayer graphene and optically accessible strongly-correlated electron states in transition metal dichalcogenide heterobilayers. Dual periodicity moiré structures (DPMS) formed in layered structures with more than two layers have been shown to lead to ferromagnetism and multiple secondary Dirac points in TBG. Whilst in principle it is possible to obtain DPMS in bilayers there has not been clear experimental evidence of this yet. In this paper we present signatures of DPMS in a t…
We report the influence of uniaxial tensile mechanical strain in the range 0-2.2% on the phonon spectra and bandstructures of monolayer and bilayer molybdenum disulfide (MoS2) two-dimensional crystals. First, we employ Raman spectroscopy to observe phonon softening with increased strain, breaking the degeneracy in the E' Raman mode of MoS2, and extract a Grüneisen parameter of ~1.06. Second, using photoluminescence spectroscopy we measure a decrease in the optical band gap of MoS2 that is roughly linear with strain, ~45 meV% strain for monolayer MoS2 and ~120 meV% strain for bilayer MoS2. Thir…
Room-temperature spin-lifetime anisotropy exceeding 60 in bilayer graphene spin valves proximity coupled to WSe$_2$
nd Institute of Physics and JARA-FIT, RWTH Aachen University（亚琛工业大学第二物理研究所和JARA-FIT）；Peter Grünberg Institute (PGI-9), Forschungszentrum Jülich（于利希研究中心彼得·格林贝格研究所（PGI-9））
Strain qualitatively changes the low-energy band structure of bilayer graphene, leading to the appearance of a pair of low-energy Dirac cones near each corner of the Brillouin zone, and a Lifshitz transition, (a saddle point in the dispersion relation) at an energy proportional to the strain [M. Mucha-Kruczynski, I.L. Aleiner, and V.I. Fal'ko, Phys. Rev. B 84, 041404 (2011)]. Here, we show that in the vicinity of the Lifshitz transition the conductance of a ballistic n-p and n-p-n junction exhibits an anomaly: a non-monotonic temperature and chemical potential dependence, with the size dependi…
The twist degree of freedom provides a powerful new tool for engineering the electrical and optical properties of van der Waals heterostructures. Here, we show that the twist angle can be used to control the spin-valley properties of transition metal dichalcogenide bilayers by changing the momentum alignment of the valleys in the two layers. Specifically, we observe that the interlayer excitons in twisted WSe$_2$/WSe$_2$ bilayers exhibit a high (>60%) degree of circular polarization (DOCP) and long valley lifetimes (>40 ns) at zero electric and magnetic fields. The valley lifetime can be tuned…
We report a study of the quantum Hall states (QHSs) sequence of holes in mono- and bilayer WSe$_2$. The QHSs sequence transitions between predominantly even and predominantly odd filling factors as the hole density is tuned in the range $1.6 - 12\times10^{12}$ cm$^{-2}$. The QHSs sequence is insensitive to the transverse electric field, and tilted magnetic field measurements reveal an insensitivity of the QHSs sequence to the in-plane magnetic field, evincing that the hole spin is locked perpendicular to the WSe$_2$ plane. These observations imply that the QHSs sequence is controlled by the Ze…
For controlling the critical electric fields of the topological phase transition in single bilayer Bi(111), we investigated topological phases in a strained system through first-principles calculations. We found a quadratic band touching semimetallic state at tensile strain $ε=0.5$%. Around this strain, the topological phase can be switched to a trivial insulator by an infinitesimal electric field. The positions at which Dirac cones appear in the electric-field-induced topological phase transition changed for the strain $ε>0.5$% and $ε<0.5$%. Our results indicate that this topological phase tr…
The Continuum Model for Uniaxially Strained Bilayer Graphene Moiré Systems
Hong Kong University of Science and Technology（香港科技大学）；Chinese University of Hong Kong (Shenzhen)（香港中文大学（深圳））；Southern University of Science and Technology（南方科技大学）
Contrasting $Γ$- and K-Valley Moiré Physics in Twisted Monolayer/Bilayer WSe$_2$
University of California, Los Angeles（加州大学洛杉矶分校）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；University of Wisconsin-Madison（威斯康星大学麦迪逊分校）；National Institute for Materials Science（国立材料研究所）
Twist angle modifies the band alignment, screening, and interlayer (IL) coupling in twisted bilayers (tBLs) of transition metal dichalcogenides. Intermediate misorientation (twist angles > 15 degrees) bilayers (BLs) offer a unique opportunity to tune excitonic behavior within these concurrent physical mechanisms but are seldom studied. In this paper, we measure many-body excitonic complexes in monolayer (ML), natural BL, and tBL WSe2. Neutral biexciton (XX) is observed in tBL, while being undetected in nonencapsulated ML and BL, demonstrating unique effects of disorder screening in tBLs. The X…
We report scanning tunneling microscopy (STM) and spectroscopy (STS) measurements of monolayer and bilayer WSe$_2$. We measure a band gap of 2.21 $\pm$ 0.08 eV in monolayer WSe$_2$, which is much larger than the energy of the photoluminescence peak indicating a large excitonic binding energy. We additionally observe significant electronic scattering arising from atomic-scale defects. Using Fourier transform STS (FT-STS), we map the energy versus momentum dispersion relations for monolayer and bilayer WSe$_2$. Further, by tracking allowed and forbidden scattering channels as a function of energ…
Orientation-tunable correlated Chern insulating states in chiral twisted double bilayer graphene proximitized by WSe2
Nanjing University（南京大学）；Hefei National Laboratory（合肥国家实验室）；Yangtze Delta Region Academy of Beijing Institute of Technology (Jiaxing)（北京理工大学长三角研究院（嘉兴））；National Institute for Materials Science（国立材料研究所）；Beijing Institute of Technology（北京理工大学）；Nanjing University of Science and Technology（南京理工大学）；Jiangsu Physical Science Research Center（江苏物理科学研究中心）
The valleys in hexagonal two-dimensional systems with broken inversion symmetry carry an intrinsic orbital magnetic moment. Despite this, such systems possess zero net magnetization unless additional symmetries are broken, since the contributions from both valleys cancel. A nonzero net magnetization can be induced through applying both uniaxial strain to break the rotational symmetry of the lattice and an in-plane electric field to break time-reversal symmetry owing to the resulting current. This creates a magnetoelectric effect whose strength is characterized by a magnetoelectric susceptibili…
We study proximity-induced spin-orbit coupling (SOC) in bilayer graphene/few-layer WSe2 heterostructure devices. Contact mode atomic force microscopy (AFM) cleaning yields ultra-clean interfaces and high-mobility devices. In a perpendicular magnetic field, we measure the quantum Hall effect to determine the Landau level structure in the presence of out-of-plane Ising and in-plane Rashba SOC. A distinct Landau level crossing pattern emerges when tuning the charge density and displacement field independently with dual gates, originating from a layer-selective SOC proximity effect. Analyzing the …
Moire-Engineered Excitonic Landscape and Phonon-Mediated Recombination in Twisted WSe2 Bilayers
Indian Institute of Technology Mandi（印度技术学院曼迪分校）；CSIR-National Physical Laboratory（印度科学工业研究理事会国家物理实验室）；Academy of Scientific and Innovative Research (AcSIR)（科学与创新研究学院）；Indian Institute of Science（印度科学学院）；National Institute of Material Science（国家物质科学研究所）
