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 angle $0.2^{\circ}$, with XX corners providing $30$\,meV deep traps for the interlayer excitons for all angles. In 3R-type bilayers, both electrons and holes are trapped in triangular "3R stacking" domains, where WX$_2$ chalcogens set over MoX$_2$ molybdenums, which act as $130$\,meV deep quantum boxes for interlayer excitons for twist angles $\lesssim 1^{\circ}$, for larger angles shifting towards domain wall network XX stacking sites.
Moiré patterns made of two-dimensional (2D) materials represent highly tunable electronic Hamiltonians, allowing a wide range of quantum phases to emerge in a single material. Current modeling techniques for moiré electrons requires significant technical work specific to each material, impeding large-scale searches for useful moiré materials. In order to address this difficulty, we have developed a material-agnostic machine learning approach and test it here on prototypical one-dimensional (1D) moiré tight-binding models. We utilize the stacking dependence of the local density of states (SD-LD…
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…
The relative orientation (twist) of successive layers of stacked two-dimensional (2D) materials creates variations in the interlayer atomic registry. The variations often form a super lattice, called a moiré pattern, which can alter electronic properties. In this work we introduce a classification of the single-particle electronic structures that can occur in twisted stacks of 2D layers by characterizing them as "moiré molecules" or "moiré crystals". The molecules generate localized electronic states and moiré flat bands, while the crystals are sometimes unconventional and produce electronic b…
We study electronic contribution to the Raman scattering signals of two-, three- and four-layer graphene with layers at one of the interfaces twisted by a small angle with respect to each other. We find that the Raman spectra of these systems feature two peaks produced by van Hove singularities in moiré minibands of twistronic graphene, one related to direct hybridization of Dirac states, and the other resulting from band folding caused by moiré superlattice. The positions of both peaks strongly depend on the twist angle, so that their detection can be used for non-invasive characterization of…
Ultra-small-angle graphene twistronics with monolayer spacers: From interlayer hybridisation and moiré effects to high-temperature magnetotransport oscillations
University of Manchester（曼彻斯特大学）；National Graphene Institute, University of Manchester（国家石墨烯研究所，曼彻斯特大学）；City University of Hong Kong（香港城市大学）；National University of Singapore（新加坡国立大学）；Institute for Functional Intelligent Materials, National University of Singapore（功能智能材料研究所，新加坡国立大学）
Spatially periodic structures with a long range period, referred to as moiré pattern, can be obtained in van der Waals bilayers in the presence of a small stacking angle or of lattice mismatch between the monolayers. Theoretical predictions suggest that the resulting spatially periodic variation of the band structure modifies the optical properties of both intra and interlayer excitons of transition metal dichalcogenides heterostructures. Here, we report on the impact of the moiré pattern formed in a MoSe$_2$/MoS$_2$ heterobilayer encapsulated in hexagonal boron nitride. The periodic in-plane …
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…
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…
We introduce a theoretical framework for the new concept of three-dimensional (3D) twistronics by developing a generalized Bloch band theory for 3D layered systems with a constant twist angle $θ$ between successive layers. Our theory employs a nonsymmorphic symmetry that enables a precise definition of an effective out-of-plane crystal momentum, and also captures the in-plane moiré pattern formed between neighboring twisted layers. To demonstrate the novel topological physics that can be achieved through 3D twistronics, we present two examples. In the first example of chiral twisted graphite, …
The recent discovery of superconductivity in magic-angle twisted bilayer graphene has sparked a renewed interest in the strongly-correlated physics of $sp^2$ carbons, in stark contrast to preliminary investigations which were dominated by the one-body physics of the massless Dirac fermions. We thus provide a self-contained, theoretical perspective of the journey of graphene from its single-particle physics-dominated regime to the strongly-correlated physics of the flat bands. Beginning from the origin of the Dirac points in condensed matter systems, we discuss the effect of the superlattice on…
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 …
Layer-Hybridized Wigner Crystals in MoSe2/WS2 Moiré Superlattice
Carnegie Mellon University（卡内基梅隆大学）；Arizona State University（亚利桑那州立大学）；National Institute for Materials Science（国立材料研究所）；The University of Texas at Dallas（德克萨斯大学达拉斯分校）；University of California at Riverside（加州大学河滨分校）
Geometrical moiré patterns, generic for almost aligned bilayers of two-dimensional (2D) crystals with similar lattice structure but slightly different lattice constants, lead to zone folding and miniband formation for electronic states. Here, we show that moiré superlattice (mSL) effects in $\mathrm{MoSe}_2/\mathrm{WS}_2$ and $\mathrm{MoTe}_2/\mathrm{MoSe}_2$ heterobilayers that feature alignment of the band edges are enhanced by resonant interlayer hybridization, and anticipate similar features in twisted homobilayers of TMDs, including examples of narrow minibands close to the actual band ed…
Transition metal dichalcogenide heterobilayers offer attractive opportunities to realize lattices of interacting bosons with several degrees of freedom. Such heterobilayers can feature moiré patterns that modulate their electronic band structure, leading to spatial confinement of single interlayer excitons (IXs) that act as quantum emitters with $C_3$ symmetry. However, the narrow emission linewidths of the quantum emitters contrast with a broad ensemble IX emission observed in nominally identical heterobilayers, opening a debate regarding the origin of IX emission. Here we report the continuo…
Layer-tunable Hubbard bands probed via moiré excitons in MoSe$_2$/WS$_2$ heterostructures
University of California, Riverside（加州大学河滨分校）；University of Southern California（南加州大学）；Tamkang University（淡江大学）；National Institute for Materials Science（日本国立材料研究所）
The creation of moiré patterns in crystalline solids is a powerful approach to manipulate their electronic properties, which are fundamentally influenced by periodic potential landscapes. In 2D materials, a moiré pattern with a superlattice potential can form by vertically stacking two layered materials with a twist and/or finite lattice constant difference. This unique approach has led to emergent electronic phenomena, including the fractal quantum Hall effect, tunable Mott insulators, and unconventional superconductivity. Furthermore, theory predicts intriguing effects on optical excitations…
Optoelectronic properties of van der Waals homostructures can be selectively engineered by the relative twist angle between layers. Here, we study the twist-dependent moire coupling in MoSe2 homobilayers. For small angles, we find a pronounced redshift of the K-K and Γ-K excitons accompanied by a transition from K-K to Γ-K emission. Both effects can be traced back to the underlying moire pattern in the MoSe2 homobilayers, as confirmed by our low-energy continuum model for different moire excitons. We identify two distinct intralayer moire excitons for R-stacking, while H-stacking yields two de…
Moiré superlattices in the twisted bilayer graphene provide an unprecedented platform to investigate a wide range of exotic quantum phenomena. Recently, the twist degree of freedom has been introduced into various classical wave systems, giving rise to new ideas for the wave control. The question is whether twistronics and moiré physics can be extended to electronics with potential applications in the twist-enabled signal processing. Here, we demonstrate both in theory and experiment that lots of fascinating moiré physics can be engineered using electric circuits with extremely high degrees of…
Moiré patterns with angular mismatch in van der Waals heterostructures composed of atomically thin semiconducting materials are a fascinating platform to engineer the optically generated excitonic properties towards novel quantum phenomena. The moiré pattern as a periodic trap potential can give rise to spatially ordered zero-dimensional (0D) exciton ensembles, which offers the possibility for dense coherent quantum emitters and quantum simulation of many-body physics. The intriguing moiré exciton properties are affected by their dynamics and exciton-phonon interaction. However, the moiré exci…
Moiré structures in small-angle-twisted bilayers of two-dimensional semiconductors with a broken-symmetry interface form arrays of ferroelectric domains with periodically alternating out-of-plane polarization. Here, we propose a network theory for the tunability of such FE domain structure by applying an electric field perpendicular to the 2D crystal. Using multiscale analysis, we derive a fully parametrized string-theory-like description of the domain wall network and show that it undergoes a qualitative change, after the arcs of partial dislocation like domain walls merge (near the network n…
Two dimensional materials and their heterostructures constitute a promising platform to study correlated electronic states as well as many body physics of excitons. Here, we present experiments that unite these hitherto separate efforts and show how excitons that are dynamically screened by itinerant electrons to form exciton-polarons, can be used as a spectroscopic tool to study interaction-induced incompressible states of electrons. The MoSe$_2$/hBN/MoSe$_2$ heterostructure that we study exhibits a long-period Moiré superlattice as evidenced by coherent-hole tunneling mediated avoided crossi…
Layered two-dimensional materials exhibit rich transport and optical phenomena in twisted or lattice-incommensurate heterostructures with spatial variations of interlayer hybridization arising from moiré interference effects. Here, we report experimental and theoretical studies of excitons in twisted heterobilayers and heterotrilayers of transition metal dichalcogenides. Using MoSe$_2$-WSe$_2$ stacks as representative realizations of twisted van der Waals bilayer and trilayer heterostructures, we observe contrasting optical signatures and interpret them in the theoretical framework of interlay…
Two-dimensional moiré materials provide a highly tunable platform to investigate strongly correlated electronic states. Such emergent many-body phenomena can be optically probed in moiré systems created by stacking two layers of transition metal dichalcogenide semiconductors: optically injected excitons can interact with itinerant carriers occupying narrow moiré bands to form exciton-polarons sensitive to strong correlations. Here, we investigate the behaviour of excitons dressed by a Fermi sea localised by the moiré superlattice of a molybdenum diselenide (MoSe$_2$) / tungsten diselenide (WSe…
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…
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…
The emerging field of twistronics, which harnesses the twist angle between two-dimensional materials, represents a promising route for the design of quantum materials, as the twist-angle-induced superlattices offer means to control topology and strong correlations. At the small twist limit, and particularly under strain, as atomic relaxation prevails, the emergent moiré superlattice encodes elusive insights into the local interlayer interaction. Here we introduce moiré metrology as a combined experiment-theory framework to probe the stacking energy landscape of bilayer structures at the 0.1 me…
Semiconductor moiré heterostructures exhibit rich correlation-induced many-body phenomena with signatures of emergent magnetism, Mott insulating states or generalized Wigner crystals observed in optical spectroscopy by probing intralayer excitons. However, as the staggered band alignment in the underlying WSe$_2$/WS$_2$ heterobilayer system separates photoexcited electrons and holes to form lowest-energy interlayer excitons, direct access to interactions between correlated charge states and ground state moiré excitons remained elusive. Here, we use MoSe$_2$/WS$_2$ heterostacks with type-I band…
Encapsulating graphene in hexagonal Boron Nitride has several advantages: the highest mobilities reported to date are achieved in this way, and precise nanostructuring of graphene becomes feasible through the protective hBN layers. Nevertheless, subtle effects may arise due to the differing lattice constants of graphene and hBN, and due to the twist angle between the graphene and hBN lattices. Here, we use a recently developed model which allows us to perform band structure and magnetotransport calculations of such structures, and show that with a proper account of the moiré physics an excelle…
We discover chiral phonons at the lowest-energy bands in moiré superlattices. The moiré chiral phonons we uncover are the collective excitations of the stacking domains. Their origin is uniquely attributed to the stacking configurations whose interlayer binding energy breaks the $C_{2z}$ symmetry on the moiré length scale. Within elastic theory, we use a general symmetry analysis to provide a complete classification of van der Waals heterostructures in respect to hosting moiré chiral phonons and show the calculation for twisted MoS$_2$ as an example. We present a low-energy effective model to …
The electronic properties of van der Waals (vdW) structures can be substantially modified by the moire superlattice potential, which strongly depends on the twist angle among the compounds. In twisted bilayer graphene (TBG), two low-energy Van Hove singularities (VHSs) move closer with decreasing twist angles and finally become highly non-dispersive flat bands at the magic angle (~ 1.1 degree). When the Fermi level lies within the flat bands of the TBG near the magic angle, Coulomb interaction is supposed to exceed the kinetic energy of the electrons, which can drive the system into various st…
Moiré superlattices - periodic orbital overlaps and lattice-reconstruction between sites of high atomic registry in vertically-stacked 2D layered materials - are quantum-active interfaces where non-trivial quantum phases on novel phenomena can emerge from geometric arrangements of 2D materials, which are not intrinsic to the parent materials. Unexpected distortions in band-structure and topology lead to long-range correlations, charge-ordering, and several other fascinating quantum phenomena hidden within the physical space between the (similar or dissimilar) parent materials. Stacking, twisti…
Moiré heterostructures are rapidly emerging as a tunable platform to study correlated electronic phenomena. Discovery of exotic quantum phases in moiré systems requires novel probes of charge and spin order. Unlike detection schemes which average over several moiré cells, local sensors can provide richer information with greater sensitivity. We study a WSe$_2$/MoSe$_2$/WSe$_2$ heterotrilayer which hosts excitons and electrons in distinct moiré lattices, and show that localized dipolar excitons are sensitive proximity charge sensors, uncovering numerous correlated electronic states at fractiona…
Polarization Vortices in a Ferromagnetic Metal via Twistronics
Beijing Institute of Technology（北京理工大学）；Catalan Institute of Nanoscience and Nanotechnology - ICN2 (CSIC & BIST)（加泰罗尼亚纳米科学和纳米技术研究所）；Autonomous University of Barcelona（巴塞罗那自治大学）；Port d' Informació Científica (PIC)（科学信息港）；Institut de Física d’Altes Energies (IFAE), The Barcelona Institute of Science and Technology (BIST)（高能物理研究所，巴塞罗那科学技术学院）；Centro de Investigaciones Energéticas, Medioambientales y Tecnológicas (CIEMAT)（能源、环境和技术研究中央中心）；State Key Laboratory of New Ceramic Materials, School of Materials Science and Engineering, Tsinghua University（清华大学材料科学与工程学院，新型陶瓷与先进工艺国家重点实验室）；Beijing Institute of Technology (Zhuhai)（北京理工大学（珠海））；Institució Catalana de Recerca i Estudis Avançats (ICREA)（加泰罗尼亚研究高级学院）
Stacking monolayers of transition metal dichalcogenides into a heterostructure with a finite twist-angle gives rise to artificial moiré superlattices with a tunable periodicity. As a consequence, excitons experience a periodic potential, which can be exploited to tailor optoelectronic properties of these materials. While recent experimental studies have confirmed twist-angle dependent optical spectra, the microscopic origin of moiré exciton resonances has not been fully clarified yet. Here, we combine first principle calculations with the excitonic density matrix formalism to study transitions…
The properties of van der Waals (vdW) heterostructures are drastically altered by a tunable moiré superlattice arising from periodic variations of atomic alignment between the layers. Exciton diffusion represents an important channel of energy transport in semiconducting transition metal dichalcogenides (TMDs). While early studies performed on TMD heterobilayers have suggested that carriers and excitons exhibit long diffusion lengths, a rich variety of scenarios can exist. In a moiré crystal with a large supercell size and deep potential, interlayer excitons may be completely localized. As the…
