Interlayer Fermi Polarons of Excited Exciton States in Quantizing Magnetic Fields.

The study of exciton polarons has offered profound insights into the many-body interactions between bosonic excitations and their immersed Fermi sea within layered heterostructures. However, little is known about the properties of exciton polarons with interlayer interactions. Here, through magneto-optical reflectance contrast measurements, we experimentally investigate interlayer Fermi polarons for 2s excitons in WSe2/graphene heterostructures, where the excited exciton states (2s) in the WSe2 layer are dressed by free charge carriers of the adjacent graphene layer in the Landau quantization regime. First, such a system enables an optical detection of integer and fractional quantum Hall states (e.g., ν = ±1/3, ±2/3) of monolayer graphene. Furthermore, we observe that the 2s state evolves into two distinct branches, denoted as attractive and repulsive polarons, when graphene is doped out of the incompressible quantum Hall gaps. Our work paves the way for the understanding of the excited composite quasiparticles and Bose-Fermi mixtures.

Evidence of the fractional quantum spin Hall effect in moiré MoTe2.

Quantum spin Hall (QSH) insulators are two-dimensional electronic materials that have a bulk band gap similar to an ordinary insulator but have topologically protected pairs of edge modes of opposite chiralities1-6. So far, experimental studies have found only integer QSH insulators with counter-propagating up-spins and down-spins at each edge leading to a quantized conductance G0 = e2/h (with e and h denoting the electron charge and Planck's constant, respectively)7-14. Here we report transport evidence of a fractional QSH insulator in 2.1° twisted bilayer MoTe2, which supports spin-Sz conservation and flat spin-contrasting Chern bands15,16. At filling factor ν = 3 of the moiré valence bands, each edge contributes a conductance 3 2 G 0 with zero anomalous Hall conductivity. The state is probably a time-reversal pair of the even-denominator 3/2-fractional Chern insulators. Furthermore, at ν = 2, 4 and 6, we observe a single, double and triple QSH insulator with each edge contributing a conductance G0, 2G0 and 3G0, respectively. Our results open up the possibility of realizing time-reversal symmetric non-abelian anyons and other unexpected topological phases in highly tunable moiré materials17-19.

Remote imprinting of moiré lattices.

Two-dimensional moiré materials are formed by overlaying two layered crystals with small differences in orientation or/and lattice constant, where their direct coupling generates moiré potentials. Moiré materials have emerged as a platform for the discovery of new physics and device concepts, but while moiré materials are highly tunable, once formed, moiré lattices cannot be easily altered. Here we demonstrate the electrostatic imprinting of moiré lattices onto a target monolayer semiconductor. The moiré potential-created by a lattice of electrons that is supported by a Mott insulator state in a remote MoSe2/WS2 moiré bilayer-imprints a moiré potential that generates flat bands and correlated insulating states in the target monolayer and can be turned on/off by gate tuning the doping density of the moiré bilayer. Additionally, we studied the interplay between the electrostatic and structural relaxation contributions to moiré imprinting. Our results demonstrate a pathway towards gate control of moiré lattices.

Giant spin Hall effect in AB-stacked MoTe2/WSe2 bilayers.

The spin Hall effect (SHE), in which an electrical current generates a 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 favours larger SHEs but shorter spin relaxation times and diffusion lengths. However, correlated magnetic materials often do not support large SHEs. Achieving large SHEs, long-range spin transport and magnetism simultaneously in a single material is attractive for spintronics applications but has remained a challenge. Here we demonstrate a giant intrinsic SHE coexisting with ferromagnetism in AB-stacked MoTe2/WSe2 moiré bilayers by direct magneto-optical imaging. Under moderate electrical currents with density <1 A m-1, we observe spin accumulation on transverse sample edges that nearly saturates the spin density. We also demonstrate long-range spin Hall transport and efficient non-local spin accumulation that is limited only by the device size (about 10 µm). The gate dependence shows that the giant SHE occurs only near the interaction-driven Chern insulating state. At low temperatures, it emerges after the quantum anomalous Hall breakdown. Our results demonstrate moiré engineering of Berry curvature and electronic correlation for potential spintronics applications.

Thermodynamic evidence of fractional Chern insulator in moiré MoTe2.

Chern insulators, which are the lattice analogues of the quantum Hall states, can potentially manifest high-temperature topological orders at zero magnetic field to enable next-generation topological quantum devices1-3. Until now, integer Chern insulators have been experimentally demonstrated in several systems at zero magnetic field3-8, whereas fractional Chern insulators have been reported in only graphene-based systems under a finite magnetic field9,10. The emergence of semiconductor moiré materials11, which support tunable topological flat bands12,13, provides an opportunity to realize fractional Chern insulators13-16. Here we report thermodynamic evidence of both integer and fractional Chern insulators at zero magnetic field in small-angle twisted bilayer MoTe2 by combining the local electronic compressibility and magneto-optical measurements. At hole filling factor ν = 1 and 2/3, the system is incompressible and spontaneously breaks time-reversal symmetry. We show that they are integer and fractional Chern insulators, respectively, from the dispersion of the state in the filling factor with an applied magnetic field. We further demonstrate electric-field-tuned topological phase transitions involving the Chern insulators. Our findings pave the way for the demonstration of quantized fractional Hall conductance and anyonic excitation and braiding17 in semiconductor moiré materials.

Quantum Oscillations in Graphene Using Surface Acoustic Wave Resonators.

Surface acoustic waves (SAWs) provide a contactless method for measuring wave-vector-dependent conductivity. This technique has been used to discover emergent length scales in the fractional quantum Hall regime of traditional, semiconductor-based heterostructures. SAWs would appear to be an ideal match for van der Waals heterostructures, but the right combination of substrate and experimental geometry to allow access to the quantum transport regime has not yet been found. We demonstrate that SAW resonant cavities fabricated on LiNbO_{3} substrates can be used to access the quantum Hall regime of high-mobility, hexagonal boron nitride encapsulated, graphene heterostructures. Our work establishes SAW resonant cavities as a viable platform for performing contactless conductivity measurements in the quantum transport regime of van der Waals materials.

Switchable moiré potentials in ferroelectric WTe2/WSe2 superlattices.

Moiré materials with superlattice periodicity many times the atomic length scale have shown strong electronic correlations and band topology with unprecedented tunability. Non-volatile control of the moiré potentials could allow on-demand switching of superlattice effects but has remained challenging to achieve. Here we demonstrate the switching of the correlated and moiré band insulating states, and the associated nonlinear anomalous Hall effect, by the ferroelectric effect. This is achieved in a ferroelectric WTe2 bilayer of the Td structure with a centred-rectangular moiré superlattice induced by interfacing with a WSe2 monolayer of the H structure. The results can be understood in terms of polarization-dependent charge transfer between two WTe2 monolayers, in which the interfacial layer has a much stronger moiré potential depth; ferroelectric switching thus turns on and off the moiré insulating states. Our study demonstrates the potential for creating new functional moiré materials by incorporating intrinsic symmetry-breaking orders.

Gate-tunable heavy fermions in a moiré Kondo lattice.

The Kondo lattice-a matrix of local magnetic moments coupled through spin-exchange interactions to itinerant conduction electrons-is a prototype of strongly correlated quantum matter1-4. Usually, Kondo lattices are realized in intermetallic compounds containing lanthanide or actinide1,2. The complex electronic structure and limited tunability of both the electron density and exchange interactions in these bulk materials pose considerable challenges to studying Kondo lattice physics. Here we report the realization of a synthetic Kondo lattice in AB-stacked MoTe2/WSe2 moiré bilayers, in which the MoTe2 layer is tuned to a Mott insulating state, supporting a triangular moiré lattice of local moments, and the WSe2 layer is doped with itinerant conduction carriers. We observe heavy fermions with a large Fermi surface below the Kondo temperature. We also observe the destruction of the heavy fermions by an external magnetic field with an abrupt decrease in the Fermi surface size and quasi-particle mass. We further demonstrate widely and continuously gate-tunable Kondo temperatures through either the itinerant carrier density or the Kondo interaction. Our study opens the possibility of in situ access to the phase diagram of the Kondo lattice with exotic quantum criticalities in a single device based on semiconductor moiré materials2-9.

Exciton density waves in Coulomb-coupled dual moiré lattices.

Strongly correlated bosons in a lattice are a platform that can realize rich bosonic states of matter and quantum phase transitions1. While strongly correlated bosons in a lattice have been studied in cold-atom experiments2-4, their realization in a solid-state system has remained challenging5. Here we trap interlayer excitons-bosons composed of bound electron-hole pairs, in a lattice provided by an angle-aligned WS2/bilayer WSe2/WS2 multilayer. The heterostructure supports Coulomb-coupled triangular moiré lattices of nearly identical period at the top and bottom interfaces. We observe correlated insulating states when the combined electron filling factor of the two lattices, with arbitrary partitions, equals [Formula: see text] and [Formula: see text]. These states can be interpreted as exciton density waves in a Bose-Fermi mixture of excitons and holes6,7. Because of the strong repulsive interactions between the constituents, the holes form robust generalized Wigner crystals8-11, which restrict the exciton fluid to channels that spontaneously break the translational symmetry of the lattice. Our results demonstrate that Coulomb-coupled moiré lattices are fertile ground for correlated many-boson phenomena12,13.

Evidence of frustrated magnetic interactions in a Wigner-Mott insulator.

Electrons in two-dimensional semiconductor moiré materials are more delocalized around the lattice sites than those in conventional solids1,2. The non-local contributions to the magnetic interactions can therefore be as important as the Anderson superexchange3, which makes the materials a unique platform to study the effects of competing magnetic interactions3,4. Here we report evidence of strongly frustrated magnetic interactions in a Wigner-Mott insulator at a two-thirds (2/3) filling of the moiré lattice in angle-aligned WSe2/WS2 bilayers. Magneto-optical measurements show that the net exchange interaction is antiferromagnetic for filling factors below 1 with a strong suppression at a 2/3 filling. The suppression is lifted on screening of the long-range Coulomb interactions and melting of the Wigner-Mott insulators by a nearby metallic gate. The results can be qualitatively captured by a honeycomb-lattice spin model with an antiferromagnetic nearest-neighbour coupling and a ferromagnetic second-neighbour coupling. Our study establishes semiconductor moiré materials as a model system for lattice-spin physics and frustrated magnetism5.

A tunable bilayer Hubbard model in twisted WSe2.

Moiré materials with flat electronic bands provide a highly controllable quantum system for studies of strong-correlation physics and topology. In particular, angle-aligned heterobilayers of semiconducting transition metal dichalcogenides with large band offset realize the single-band Hubbard model. Introduction of a new layer degree of freedom is expected to foster richer interactions, enabling Hund's physics, interlayer exciton condensation and new superconducting pairing mechanisms to name a few. Here we report competing electronic states in twisted AB-homobilayer WSe2, which realizes a bilayer Hubbard model in the weak interlayer hopping limit for holes. By layer-polarizing holes via a perpendicular electric field, we observe a crossover from an excitonic insulator to a charge-transfer insulator at a hole density of ν = 1 (in units of moiré density), a transition from a paramagnetic to an antiferromagnetic charge-transfer insulator at ν = 2 and evidence for a layer-selective Mott insulator at 1 < ν < 2. The unique coupling of charge and spin to external electric and magnetic fields also manifests a giant magnetoelectric response. Our results establish a new solid-state simulator for the bilayer Hubbard model Hamiltonian.

Dielectric catastrophe at the Wigner-Mott transition in a moiré superlattice.

The bandwidth-tuned Wigner-Mott transition is an interaction-driven phase transition from a generalized Wigner crystal to a Fermi liquid. Because the transition is generally accompanied by both magnetic and charge-order instabilities, it remains unclear if a continuous Wigner-Mott transition exists. Here, we demonstrate bandwidth-tuned metal-insulator transitions at fixed fractional fillings of a MoSe2/WS2 moiré superlattice. The bandwidth is controlled by an out-of-plane electric field. The dielectric response is probed optically with the 2s exciton in a remote WSe2 sensor layer. The exciton spectral weight is negligible for the metallic state with a large negative dielectric constant. It continuously vanishes when the transition is approached from the insulating side, corresponding to a diverging dielectric constant or a 'dielectric catastrophe' driven by the critical charge dynamics near the transition. Our results support the scenario of continuous Wigner-Mott transitions in two-dimensional triangular lattices and stimulate future explorations of exotic quantum phases in their vicinities.

Semiconductor moiré materials.

Moiré materials have emerged as a platform for exploring the physics of strong electronic correlations and non-trivial band topology. Here we review the recent progress in semiconductor moiré materials, with a particular focus on transition metal dichalcogenides. Following a brief overview of the general features in this class of materials, we discuss recent theoretical and experimental studies on Hubbard physics, Kane-Mele-Hubbard physics and equilibrium moiré excitons. We also comment on the future opportunities and challenges in the studies of transition metal dichalcogenide and other semiconductor moiré materials.

van der Waals π Josephson Junctions.

Proximity-induced superconductivity in a ferromagnet can induce Cooper pairs with a finite center-of-mass momentum and stabilize Josephson junctions (JJs) with π phase difference in superconductor-ferromagnet-superconductor heterostructures. The emergence of two-dimensional layered superconducting and magnetic materials promises a new platform for realizing π JJs with atomically sharp interfaces. Here we demonstrate a thickness-driven 0-π transition in JJs made of NbSe2 (an Ising superconductor) and Cr2Ge2Te6 (a ferromagnetic semiconductor). By systematically increasing the Cr2Ge2Te6 weak link thickness, we observe a vanishing supercurrent at a critical thickness of ∼8 nm, followed by a re-entrant supercurrent. Near the critical thickness, we further observe unusual supercurrent interference patterns with vanishing critical current around zero in-plane magnetic field. They signify the formation of 0-π JJs (with both 0 and π regions), likely induced by the nanoscale magnetic domains in Cr2Ge2Te6.

Strong interlayer interactions in bilayer and trilayer moiré superlattices.

Moiré superlattices constructed from transition metal dichalcogenides have demonstrated a series of emergent phenomena, including moiré excitons, flat bands, and correlated insulating states. All of these phenomena depend crucially on the presence of strong moiré potentials, yet the properties of these moiré potentials, and the mechanisms by which they can be generated, remain largely open questions. Here, we use angle-resolved photoemission spectroscopy with submicron spatial resolution to investigate an aligned WS2/WSe2 moiré superlattice and graphene/WS2/WSe2 trilayer heterostructure. Our experiments reveal that the hybridization between moiré bands in WS2/WSe2 exhibits an unusually large momentum dependence, with the splitting between moiré bands at the Γ point more than an order of magnitude larger than that at K point. In addition, we discover that the same WS2/WSe2 superlattice can imprint an unexpectedly large moiré potential on a third, separate layer of graphene (g/WS2/WSe2), suggesting new avenues for engineering two-dimensional moiré superlattices.

Reproducibility in the fabrication and physics of moiré materials.

Overlaying two atomic layers with a slight lattice mismatch or at a small rotation angle creates a moiré superlattice, which has properties that are markedly modified from (and at times entirely absent in) the 'parent' materials. Such moiré materials have progressed the study and engineering of strongly correlated phenomena and topological systems in reduced dimensions. The fundamental understanding of the electronic phases, such as superconductivity, requires a precise control of the challenging fabrication process, involving the rotational alignment of two atomically thin layers with an angular precision below 0.1 degrees. Here we review the essential properties of moiré materials and discuss their fabrication and physics from a reproducibility perspective.

Valley-Polarized Quantum Anomalous Hall State in Moiré MoTe_{2}/WSe_{2} Heterobilayers.

Moiré heterobilayer transition metal dichalcogenides (TMDs) emerge as an ideal system for simulating the single-band Hubbard model and interesting correlated phases have been observed in these systems. Nevertheless, the moiré bands in heterobilayer TMDs were believed to be topologically trivial. Recently, it was reported that both a quantum valley Hall insulating state at filling ν=2 (two holes per moiré unit cell) and a valley-polarized quantum anomalous Hall state at filling ν=1 were observed in AB stacked moiré MoTe_{2}/WSe_{2} heterobilayers. However, how the topologically nontrivial states emerge is not known. In this Letter, we propose that the pseudomagnetic fields induced by lattice relaxation in moiré MoTe_{2}/WSe_{2} heterobilayers could naturally give rise to moiré bands with finite Chern numbers. We show that a time-reversal invariant quantum valley Hall insulator is formed at full filling ν=2, when two moiré bands with opposite Chern numbers are filled. At half filling ν=1, the Coulomb interaction lifts the valley degeneracy and results in a valley-polarized quantum anomalous Hall state, as observed in the experiment. Our theory identifies a new way to achieve topologically nontrivial states in heterobilayer TMD materials.

Coexisting ferromagnetic-antiferromagnetic state in twisted bilayer CrI3.

Moiré engineering1-3 of van der Waals magnetic materials4-9 can yield new magnetic ground states via competing interactions in moiré superlattices10-13. Theory predicts a suite of interesting phenomena, including multiflavour magnetic states10, non-collinear magnetic states10-13, moiré magnon bands and magnon networks14 in twisted bilayer magnetic crystals, but so far such non-trivial magnetic ground states have not emerged experimentally. Here, by utilizing the stacking-dependent interlayer exchange interactions in two-dimensional magnetic materials15-18, we demonstrate a coexisting ferromagnetic (FM) and antiferromagnetic (AF) ground state in small-twist-angle CrI3 bilayers. The FM-AF state transitions to a collinear FM ground state above a critical twist angle of about 3°. The coexisting FM and AF domains result from a competition between the interlayer AF coupling, which emerges in the monoclinic stacking regions of the moiré superlattice, and the energy cost for forming FM-AF domain walls. Our observations are consistent with the emergence of a non-collinear magnetic ground state with FM and AF domains on the moiré length scale10-13. We further employ the doping dependence of the interlayer AF interaction to control the FM-AF state by electrically gating a bilayer sample. These experiments highlight the potential to create complex magnetic ground states in twisted bilayer magnetic crystals, and may find application in future gate-voltage-controllable high-density magnetic memory storage.

Quantum anomalous Hall effect from intertwined moiré bands.

Electron correlation and topology are two central threads of modern condensed matter physics. Semiconductor moiré materials provide a highly tuneable platform for studies of electron correlation1-12. Correlation-driven phenomena, including the Mott insulator2-5, generalized Wigner crystals2,6,9, stripe phases10 and continuous Mott transition11,12, have been demonstrated. However, non-trivial band topology has remained unclear. Here we report the observation of a quantum anomalous Hall effect in AB-stacked MoTe2 /WSe2 moiré heterobilayers. Unlike in the AA-stacked heterobilayers11, an out-of-plane electric field not only controls the bandwidth but also the band topology by intertwining moiré bands centred at different layers. At half band filling, corresponding to one particle per moiré unit cell, we observe quantized Hall resistance, h/e2 (with h and e denoting the Planck's constant and electron charge, respectively), and vanishing longitudinal resistance at zero magnetic field. The electric-field-induced topological phase transition from a Mott insulator to a quantum anomalous Hall insulator precedes an insulator-to-metal transition. Contrary to most known topological phase transitions13, it is not accompanied by a bulk charge gap closure. Our study paves the way for discovery of emergent phenomena arising from the combined influence of strong correlation and topology in semiconductor moiré materials.

Quantum Oscillations in Two-Dimensional Insulators Induced by Graphite Gates.

We demonstrate a mechanism for magnetoresistance oscillations in insulating states of two-dimensional (2D) materials arising from the interaction of the 2D layer and proximal graphite gates. We study a series of devices based on different 2D systems, including mono- and bilayer T_{d}-WTe_{2}, MoTe_{2}/WSe_{2} moiré heterobilayers, and Bernal-stacked bilayer graphene, which all share a similar graphite-gated geometry. We find that the 2D systems, when tuned near an insulating state, generically exhibit magnetoresistance oscillations corresponding to a high-density Fermi surface, in contravention of naïve band theory. Simultaneous measurement of the resistivity of the graphite gates shows that the oscillations of the sample layer are precisely correlated with those of the graphite gates. Further supporting this connection, the oscillations are quenched when the graphite gate is replaced by a low-mobility metal, TaSe_{2}. The observed phenomenon arises from the oscillatory behavior of graphite density of states, which modulates the device capacitance and, as a consequence, the carrier density in the sample layer even when a constant electrochemical potential is maintained between the sample and the gate electrode. Oscillations are most pronounced near insulating states where the resistivity is strongly density dependent. Our study suggests a unified mechanism for quantum oscillations in graphite-gated 2D insulators based on electrostatic sample-gate coupling.