We study the edge states of twisted bilayer graphene and their topological origin. We show that the twisted bilayer graphene has special edge states associated with the moiré pattern, and the emergence of these moiré edge states is linked with the sliding Chern number, which describes topological charge pumping caused by relative interlayer sliding. When one layer of the twisted bilayer is relatively slid with respect to the other layer, the edge states are transferred from a single band to another across the band gap, and the number of the edge states pumped in a sliding cycle is shown to be equal to the sliding Chern number of the band gap. The relationship can be viewed as a manifestation of the bulk-edge correspondence inherent in moiré bilayer systems.
We study the adiabatic topological charge pumping driven by interlayer sliding in the moiré superlattices. We show that, when we slide a single layer of the twisted bilayer system relatively to the other, a moiré pattern flow and a quantized transport of electrons occurs. When the Fermi energy is in a spectral gap, the number of pumped charges in the interlayer sliding process is quantized to a sliding Chern number, which obeys a Diophantine equation analogous to the quantum Hall effect. We apply the argument to the twisted bilayer graphene, and find that energy gaps above and below the nearly…
In twisted bilayers of semiconducting transition metal dichalcogenides (TMDs), a combination of structural rippling and electronic coupling gives rise to periodic moiré potentials that can confine charged and neutral excitations. Here, we report experimental measurements of the structure and spectroscopic properties of twisted bilayers of WSe2 and MoSe2 in the H-stacking configuration using scanning tunneling microscopy (STM). Our experiments reveal that the moiré potential in these bilayers at small angles is unexpectedly large, reaching values of above 300 meV for the valence band and 150 me…
Moiré superlattice created by twist stacking has multiple physical properties. These physical properties depend on the twist angle, hence investigation of the twist angle dependency is important for the deep understanding of physical phenomena in moiré superlattice. In this work, negative magnetoresistance owing to weak localization (WL) was investigated in twisted double bilayer graphene (TDBG) as a function of the twist angle. The ratio of the intervalley scattering time to the intravalley scattering time, estimated using the WL formula for bilayer graphene, tended to decrease as the twist a…
Low-energy moiré flat bands in magic-angle twisted bilayer graphene (tBG) have demonstrated incredible potentials to exhibit rich exotic quantum phenomena. Theoretically, the moiré flat bands of tBG are based on the extended structures, i.e., the moiré patterns with periodic boundary conditions. However, a fundamental question of whether the flat bands can exist in the graphene moiré patterns with a reduced structure symmetry, such as sample edges, remains unanswered. Here, via scanning tunneling microscopy and spectroscopy, we study the local electronic properties of a magic-angle tBG near th…
Moiré superlattices (MSL) formed in angle-aligned bilayers of van der Waals materials have become a promising platform to realize novel two-dimensional electronic states. Angle-aligned trilayer structures can form two sets of MSLs which could potentially interfere with each other. In this work, we directly image the moiré patterns in both monolayer graphene aligned on hBN and twisted bilayer graphene aligned on hBN, using combined scanning microwave impedance microscopy and conductive atomic force microscopy. Correlation of the two techniques reveals the contrast mechanism for the achieved ult…
We construct an analytic continuum model to describe the electronic structure and the electron-phonon interaction in twisted bilayer graphenes with arbitrary lattice deformation. Starting from the tight-binding model, we derive the interlayer Hamiltonian in the presence of general lattice displacement, and obtain a long-wavelength continuum expression for smooth deformation. We show that the continuum model correctly describes the band structures of the lattice-relaxed twisted bilayer graphenes. We apply the formula to the phonon vibration, and derive an explicit expression of the electron-pho…
We study the in-plane acoustic phonons in twisted bilayer graphenes using the effective continuum approach. We calculate the phonon modes by solving the continuum equation of motion for infinitesimal vibration around the static relaxed state with triangular domain structure. We find that the moiré interlayer potential only affects the in-plane asymmetric modes, where the original linear dispersion is broken down into miniphonon bands separated by gaps, while the in-plane symmetric modes with their linear dispersion are hardly affected. The phonon wave functions of asymmetric modes are regarded…
When using hexagonal boron-nitride (hBN) as a substrate for graphene, the resulting moiré pattern creates secondary Dirac points. By encapsulating a multilayer graphene within aligned hBN sheets the controlled moiré stacking may offer even richer benefits. Using advanced tight-binding simulations on atomistically-relaxed heterostructures, here we show that the gap at the secondary Dirac point can be opened in selected moiré-stacking configurations, and is independent of any additional vertical gating of the heterostructure. On the other hand, gating can broadly tune the gap at the principal Di…
We theoretically study the electronic structure of magic-angle twisted bilayer graphene with disordered moiré patterns. By using an extended continuum model incorporating non-uniform lattice distortion, we find that the local density of states of the flat band is hardly broadened, but splits into upper and lower subbands in most places. The spatial dependence of the splitting energy is almost exclusively determined by the local value of the effective vector potential induced by heterostrain, whereas the variation of local twist angle and local moiré period give relatively minor effects on the …
Recent measurements in several different laboratories report the observation of an approximately linear-in-temperature resistivity with a large twist-angle-dependent slope (or temperature coefficient) in moiré twisted bilayer graphene (tBLG) down to a few K and sometimes to much lower temperatures. In this note, we theoretically discuss this `strange metal' linear-in-temperature transport behavior from the perspective of resistive scattering by acoustic phonons, emphasizing the aspects of the transport data, which are and which are not consistent with the phonon scattering mechanism. Extensive…
While a typical material exhibits field induced currents only at the boundary, a uniform out-of-plane magnetic field applied to two mutually rotated layers of graphene is shown to result in an ordered array of permanent current loops throughout the material. Each current loop consists of an interlayer current flowing through the open AA stacked regions of the moiré created by rotation, which then flows back through the neighboring AB regions to form a circuit, with significant current strength even at small fields. Similar moiré ordered arrays of current loops are also shown to exist in non-eq…
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…
A new implementation of stochastic many-body perturbation theory for periodic 2D systems is presented. The method is used to compute quasiparticle excitations in twisted bilayer phosphorene. Excitation energies are studied using stochastic $G_0W_0$ and partially self-consistent $\bar ΔGW_0$ approaches. The approach is inexpensive; it is used to study twisted systems with unit cells containing $>2,700$ atoms ($>13,500$ valence electrons), which corresponds to a minimum twisting angle of $\approx 3.1^\circ$. Twisted bilayers exhibit band splitting, increased localization and formation of localiz…
Moiré superlattices formed in van der Waals bilayers have enabled the creation and manipulation of new quantum states, as is exemplified by the discovery of superconducting and correlated insulating states in twisted bilayer graphene near the magic angle. Twisted bilayer semiconductors may lead to tunable exciton lattices and topological states, yet signatures of moiré excitons have been reported only in closely angularly-aligned bilayers. Here we report tuning of moiré lattice in WS$_{2}$ /MoSe$_{2}$ bilayers over a wide range of twist angles, leading to the continuous tuning of moiré lattice…
Intercalation of lithium atoms between layers of 2D materials can alter their atomic and electronic structure. We investigate effects of Li intercalation in twisted bilayers of the transition metal dichalcogenide MoS$_2$ through first-principles calculations, tight-binding parameterization based on the Wannier transformation, and analysis of moiré band structures through an effective continuum model. The energetic stability of different intercalation sites for Li between layers of MoS$_2$ are classified according to the local coordination type and the number of vertically aligned Mo atoms, sug…
Moiré enabled spin pumping and preservation in MoSe2/WS2 heterobilayers
Stanford University（斯坦福大学）；SLAC National Accelerator Laboratory（SLAC国家加速器实验室）；National Institute for Materials Science（国立材料研究所）；University of Cambridge（剑桥大学）
We consider twisted bilayer and trilayer graphene in the presence of Rashba spin-orbit coupling and explore the physics of Moiré spintronics. The electronic charge density has a sharp step right at the magic angles $θ_m$. As a result, local spin observables (polarization and equilibrium spin currents) have sharp peaks (of width about a small fraction of 1$^\circ$) as a function of the twist angle $θ$, and abrupt sign reversals at $θ_m$. Thereby, the magic angle can be determined in an unprecedented accuracy. In the first chiral limit, the spin currents vanish, but the peculiar pattern of the p…
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…
Twisted bilayer graphene (tBLG) forms a quasicrystal whose structural and electronic properties depend on the angle of rotation between its layers. Here we present a scanning tunneling microscopy study of gate-tunable tBLG devices supported by atomically-smooth and chemically inert hexagonal boron nitride (BN). The high quality of these tBLG devices allows identification of coexisting moiré patterns and moiré super-superlattices produced by graphene-graphene and graphene-BN interlayer interactions. Furthermore, we examine additional tBLG spectroscopic features in the local density of states be…
The discovery of unconventional ferroelectric behavior in twisted bilayers has prompted the consideration of moiré heterostructures as polar materials. However, misconceptions about the nature and origin of the observed ferroelectricity indicate that a better theoretical understanding of the polar properties of moiré heterostructures is needed. In this paper, it is proposed, and verified with first-principles calculations, that all moiré heterostructures exhibit an out-of-plane moiré polar domain (MPD) structure. In transition metal dichalcogenide bilayers, an interlayer charge transfer occurs…
To realize the applicative potential of 2D twistronic devices, scalable synthesis and assembly techniques need to meet stringent requirements in terms of interface cleanness and twist-angle homogeneity. Here, we show that small-angle twisted bilayer graphene assembled from separated CVD-grown graphene single-crystals can ensure high-quality transport properties, determined by a device-scale-uniform moireé potential. Via low-temperature dual-gated magnetotransport, we demonstrate the hallmarks of a $2.4^\circ$ -twisted superlattice, including tunable regimes of interlayer coupling, reduced Ferm…
Spontaneous orbital magnetism observed in twisted bilayer graphene (tBG) on nearly aligned hexagonal boron nitride (BN) substrate builds on top of the electronic structure resulting from combined G/G and G/BN double moire interfaces. Here we show that tBG/BN commensurate double moire patterns can be classified into two types, each favoring the narrowing of either the conduction or valence bands on average, and obtain the evolution of the bands as a function of the interlayer sliding vectors and electric fields. Finite valley Chern numbers $\pm 1$ are found in a wide range of parameter space wh…
We report on the theoretical electronic spectra of twisted phosphorene bilayers exhibiting moiré patterns, as computed by means of a continuous approximation to the moiré superlattice Hamiltonian. Our model is constructed by interpolating between effective $Γ$-point conduction- and valence-band Hamiltonians for the different stacking configurations approximately realized across the moiré supercell, formulated on symmetry grounds. We predict the realization of three distinct regimes for $Γ$-point electrons and holes at different twist angle ranges: a Hubbard regime for small twist angles $θ< 2^…
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）
In stacks of two-dimensional crystals, mismatch of their lattice constants and misalignment of crystallographic axes lead to formation of moiré patterns. We show that moiré superlattice effects persist in twisted bilayer graphene (tBLG) with large twists and short moiré periods. Using angle-resolved photoemission, we observe dramatic changes in valence band topology across large regions of the Brillouin zone, including the vicinity of the saddle point at $M$ and across 3 eV from the Dirac points. In this energy range, we resolve several moiré minibands and detect signatures of secondary Dirac …
The quantum anomalous Hall (QAH) effect is sometimes observed in twisted bilayer graphene (tBG) when it is nearly aligned with an encapsulating hexagonal boron nitride (hBN) layer. We propose that the appearance or absence of the QAH effect in individual devices could be related to commensurability between the graphene/graphene and graphene/hBN moiré patterns. We identify a series of points in the $(θ_{\rm GG},θ_{\rm GBN})$ twist-angle space at which the two moiré patterns are commensurate, allowing moiré band theory to be applied, and show that the band Chern numbers are in this case sensitiv…
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）
A two-dimensional (2D) hetero-bilayer system consisting of MoS2 on WSe2, deposited on epitaxial graphene, is studied by scanning tunneling microscopy and spectroscopy at temperatures of 5 and 80 K. A moiré pattern is observed, arising from lattice mismatch of 3.7% between the MoS2 and WSe2. Significant energy shifts are observed in tunneling spectra observed at the maxima of the moiré corrugation, as compared with spectra obtained at corrugation minima, consistent with prior work. Furthermore, at the minima of the moiré corrugation, sharp peaks in the spectra at energies near the band edges ar…
Aharonov-Bohm (AB) effect, the well-known archetype of electron-wave interference phenomena, has been explored extensively through transport measurements. However, these techniques lack spatial resolution that would be indispensable for studying the magnetic and electrostatic AB oscillations at the nanometer scale. Here, we demonstrated that scanning tunneling microscopy (STM) can be used as an AB interferometer operating on nanometer length scales and the magneto-electric Aharonov-Bohm effect in minimally twisted bilayer graphene (TBG) was directly measured by using STM. In the minimally TBG,…
It is widely known that the twisted bilayer graphene (TBG) shows flat bands at magic angles, which can be well described by the effective continuum model derived by Bistritzer and MacDonald (BM). We propose in this paper a similar twisted bilayer system but defined on the square lattice with $π$-flux per plaquette, and study its spectrum using the BM Hamiltonian with a mass term which is originated from the staggered potential. The basic difference between the TBG and the present model is simply rotational symmetry, $C_3$ vs $C_4$, as well as a mass term. Nevertheless, the feature of the flat …
Moiré superlattices of van der Waals heterostructures provide a powerful new way to engineer the electronic structures of two-dimensional (2D) materials. Many novel quantum phenomena have emerged in different moiré heterostructures, such as correlated insulators, superconductors, and Chern insulators in graphene systems and moiré excitons in transition metal dichalcogenide (TMDC) systems. Twisted phosphorene offers another attractive system to explore moiré physics because phosphorene features an anisotropic rectangular lattice, different from the isotropic hexagonal lattice in graphene and TM…
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…
Moiré patterns on Highly Oriented Pyrolytic Graphite surfaces due to dislocated graphene layers were studied. We observed that the apparent corrugations of the moiré patterns in scanning tunnelling microscopy images change as a function of tunnel junction bias. A simple geometric investigation of the atomic structure of the graphene layers generating moiré patterns revealed that different atomic arrangements due to different twist angles can result in similar geometric moiré periods such that, only a small fraction of the observed moiré periodicities may coincide with the real atomic periodici…
We systematically measured the DC voltage V_ISH induced by spin pumping together with the inverse spin Hall effect in ferromagnet/platinum bilayer films. In all our samples, comprising ferromagnetic 3d transition metals, Heusler compounds, ferrite spinel oxides, and magnetic semiconductors, V_ISH invariably has the same polarity. V_ISH furthermore scales with the magnetization precession cone angle with a universal prefactor, irrespective of the magnetic properties, the charge carrier transport mechanism or type. These findings quantitatively corroborate the present theoretical understanding o…
In twisted bilayer graphene, long-wavelength lattice fluctuations on the scale of the moiré period are dominated by phason modes, i.e., acoustic branches of the incommensurate lattice resulting from coherent superpositions of optical phonons. In the limit of small twist angles, these modes describe the sliding motion of stacking domain walls separating regions of partial commensuration. The resulting soliton network is a soft elastic manifold, whose reduced rigidity arises from the competition between intralayer (elastic) and interlayer (adhesion) forces governing lattice relaxation. Shear def…
Recent advances in the field of vertically stacked 2D materials have revealed a rich exciton landscape. In particular, it has been demonstrated that out-of-plane electrical fields can be used to tune the spectral position of spatially separated interlayer excitons. Other studies have shown that there is a strong hybridization of exciton states, resulting from the mixing of electronic states in both layers. However, the connection between the twist-angle dependent hybridization and field-induced energy shifts has remained in the dark. Here, we investigate on a microscopic footing the interplay …
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 study the magneto-optical conductivity of a number of Van der Waals heterostructures, namely, twisted bilayer graphene, AB-AB and AB-BA stacked twisted double bilayer graphene and monolayer graphene and AB-stacked bilayer graphene on hexagonal boron nitride. As magnetic field increases, the absorption spectrum exhibits a self-similar recursive pattern reflecting the fractal nature of the energy spectrum. Whilst twisted bilayer graphene displays only weak circular dichroism, monolayer graphene and AB-stacked bilayer graphene on hexagonal boron nitride show specifically strong circular dichro…
