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.

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.

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.

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.

Strongly correlated excitonic insulator in atomic double layers.

Excitonic insulators (EIs) arise from the formation of bound electron-hole pairs (excitons)1,2 in semiconductors and provide a solid-state platform for quantum many-boson physics3-8. Strong exciton-exciton repulsion is expected to stabilize condensed superfluid and crystalline phases by suppressing both density and phase fluctuations8-11. Although spectroscopic signatures of EIs have been reported6,12-14, conclusive evidence for strongly correlated EI states has remained elusive. Here we demonstrate a strongly correlated two-dimensional (2D) EI ground state formed in transition metal dichalcogenide (TMD) semiconductor double layers. A quasi-equilibrium spatially indirect exciton fluid is created when the bias voltage applied between the two electrically isolated TMD layers is tuned to a range that populates bound electron-hole pairs, but not free electrons or holes15-17. Capacitance measurements show that the fluid is exciton-compressible but charge-incompressible-direct thermodynamic evidence of the EI. The fluid is also strongly correlated with a dimensionless exciton coupling constant exceeding 10. We construct an exciton phase diagram that reveals both the Mott transition and interaction-stabilized quasi-condensation. Our experiment paves the path for realizing exotic quantum phases of excitons8, as well as multi-terminal exciton circuitry for applications18-20.

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.

Continuous Mott transition in semiconductor moiré superlattices.

The evolution of a Landau Fermi liquid into a non-magnetic Mott insulator with increasing electronic interactions is one of the most puzzling quantum phase transitions in physics1-6. The vicinity of the transition is believed to host exotic states of matter such as quantum spin liquids4-7, exciton condensates8 and unconventional superconductivity1. Semiconductor moiré materials realize a highly controllable Hubbard model simulator on a triangular lattice9-22, providing a unique opportunity to drive a metal-insulator transition (MIT) via continuous tuning of the electronic interactions. Here, by electrically tuning the effective interaction strength in MoTe2/WSe2 moiré superlattices, we observe a continuous MIT at a fixed filling of one electron per unit cell. The existence of quantum criticality is supported by the scaling collapse of the resistance, a continuously vanishing charge gap as the critical point is approached from the insulating side, and a diverging quasiparticle effective mass from the metallic side. We also observe a smooth evolution of the magnetic susceptibility across the MIT and no evidence of long-range magnetic order down to ~5% of the Curie-Weiss temperature. This signals an abundance of low-energy spinful excitations on the insulating side that is further corroborated by the Pomeranchuk effect observed on the metallic side. Our results are consistent with the universal critical theory of a continuous Mott transition in two dimensions4,23.

Correlated insulating states at fractional fillings of moiré superlattices.

Quantum particles on a lattice with competing long-range interactions are ubiquitous in physics; transition metal oxides1,2, layered molecular crystals3 and trapped-ion arrays4 are a few examples. In the strongly interacting regime, these systems often show a rich variety of quantum many-body ground states that challenge theory2. The emergence of transition metal dichalcogenide moiré superlattices provides a highly controllable platform in which to study long-range electronic correlations5-12. Here we report an observation of nearly two dozen correlated insulating states at fractional fillings of tungsten diselenide/tungsten disulfide moiré superlattices. This finding is enabled by a new optical sensing technique that is based on the sensitivity to the dielectric environment of the exciton excited states in a single-layer semiconductor of tungsten diselenide. The cascade of insulating states shows an energy ordering that is nearly symmetric about a filling factor of half a particle per superlattice site. We propose a series of charge-ordered states at commensurate filling fractions that range from generalized Wigner crystals7 to charge density waves. Our study lays the groundwork for using moiré superlattices to simulate a wealth of quantum many-body problems that are described by the two-dimensional extended Hubbard model3,13,14 or spin models with long-range charge-charge and exchange interactions15,16.

Simulation of Hubbard model physics in WSe2/WS2 moiré superlattices.

The Hubbard model, formulated by physicist John Hubbard in the 1960s1, is a simple theoretical model of interacting quantum particles in a lattice. The model is thought to capture the essential physics of high-temperature superconductors, magnetic insulators and other complex quantum many-body ground states2,3. Although the Hubbard model provides a greatly simplified representation of most real materials, it is nevertheless difficult to solve accurately except in the one-dimensional case2,3. Therefore, the physical realization of the Hubbard model in two or three dimensions, which can act as an analogue quantum simulator (that is, it can mimic the model and simulate its phase diagram and dynamics4,5), has a vital role in solving the strong-correlation puzzle, namely, revealing the physics of a large number of strongly interacting quantum particles. Here we obtain the phase diagram of the two-dimensional triangular-lattice Hubbard model by studying angle-aligned WSe2/WS2 bilayers, which form moiré superlattices6 because of the difference between the lattice constants of the two materials. We probe the charge and magnetic properties of the system by measuring the dependence of its optical response on an out-of-plane magnetic field and on the gate-tuned carrier density. At half-filling of the first hole moiré superlattice band, we observe a Mott insulating state with antiferromagnetic Curie-Weiss behaviour, as expected for a Hubbard model in the strong-interaction regime2,3,7-9. Above half-filling, our experiment suggests a possible quantum phase transition from an antiferromagnetic to a weak ferromagnetic state at filling factors near 0.6. Our results establish a new solid-state platform based on moiré superlattices that can be used to simulate problems in strong-correlation physics that are described by triangular-lattice Hubbard models.

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.

Evidence of high-temperature exciton condensation in two-dimensional atomic double layers.

A Bose-Einstein condensate is the ground state of a dilute gas of bosons, such as atoms cooled to temperatures close to absolute zero1. With much smaller mass, excitons (bound electron-hole pairs) are expected to condense at considerably higher temperatures2-7. Two-dimensional van der Waals semiconductors with very strong exciton binding are ideal systems for the study of high-temperature exciton condensation. Here we study electrically generated interlayer excitons in MoSe2-WSe2 atomic double layers with a density of up to 1012 excitons per square centimetre. The interlayer tunnelling current depends only on the exciton density, which is indicative of correlated electron-hole pair tunnelling8. Strong electroluminescence arises when a hole tunnels from WSe2 to recombine with an electron in MoSe2. We observe a critical threshold dependence of the electroluminescence intensity on exciton density, accompanied by super-Poissonian photon statistics near the threshold, and a large electroluminescence enhancement with a narrow peak at equal electron and hole densities. The phenomenon persists above 100 kelvin, which is consistent with the predicted critical condensation temperature9-12. Our study provides evidence for interlayer exciton condensation in two-dimensional atomic double layers and opens up opportunities for exploring condensate-based optoelectronics and exciton-mediated high-temperature superconductivity13.

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.

Tuning Exciton Emission via Ferroelectric Polarization at a Heterogeneous Interface between a Monolayer Transition Metal Dichalcogenide and a Perovskite Oxide Membrane.

We demonstrate the integration of a thin BaTiO3 (BTO) membrane with monolayer MoSe2 in a dual-gate device that enables in situ manipulation of the BTO ferroelectric polarization with a voltage pulse. While two-dimensional (2D) transition metal dichalcogenides (TMDs) offer remarkable adaptability, their hybrid integration with other families of functional materials beyond the realm of 2D materials has been challenging. Released functional oxide membranes offer a solution for 2D/3D integration via stacking. 2D TMD excitons can serve as a local probe of the ferroelectric polarization in BTO at a heterogeneous interface. Using photoluminescence (PL) of MoSe2 excitons to optically read out the doping level, we find that the relative population of charge carriers in MoSe2 depends sensitively on the ferroelectric polarization. This finding points to a promising avenue for future-generation versatile sensing devices with high sensitivity, fast readout, and diverse applicability for advanced signal processing.

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.

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.

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.

Creation of moiré bands in a monolayer semiconductor by spatially periodic dielectric screening.

Moiré superlattices of two-dimensional van der Waals materials have emerged as a powerful platform for designing electronic band structures and discovering emergent physical phenomena. A key concept involves the creation of long-wavelength periodic potential and moiré bands in a crystal through interlayer electronic hybridization or atomic corrugation when two materials are overlaid. Here we demonstrate a new approach based on spatially periodic dielectric screening to create moiré bands in a monolayer semiconductor. This approach relies on reduced dielectric screening of the Coulomb interactions in monolayer semiconductors and their environmental dielectric-dependent electronic band structure. We observe optical transitions between moiré bands in monolayer WSe2 when it is placed close to small-angle-misaligned graphene on hexagonal boron nitride. The moiré bands are a result of long-range Coulomb interactions, which are strongly gate tunable, and can have versatile superlattice symmetries independent of the crystal lattice of the host material. Our result also demonstrates that monolayer semiconductors are sensitive local dielectric sensors.

Stripe phases in WSe2/WS2 moiré superlattices.

Stripe phases, in which the rotational symmetry of charge density is spontaneously broken, occur in many strongly correlated systems with competing interactions1-11. However, identifying and studying such stripe phases remains challenging. Here we uncover stripe phases in WSe2/WS2 moiré superlattices by combining optical anisotropy and electronic compressibility measurements. We find strong electronic anisotropy over a large doping range peaked at 1/2 filling of the moiré superlattice. The 1/2 state is incompressible and assigned to an insulating stripe crystal phase. Wide-field imaging reveals domain configurations with a preferential alignment along the high-symmetry axes of the moiré superlattice. Away from 1/2 filling, we observe additional stripe crystals at commensurate filling 1/4, 2/5 and 3/5, and compressible electronic liquid crystal states at incommensurate fillings. Our results demonstrate that two-dimensional semiconductor moiré superlattices are a highly tunable platform from which to study the stripe phases and their interplay with other symmetry breaking ground states.

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.

Evolution of interlayer and intralayer magnetism in three atomically thin chromium trihalides.

We conduct a comprehensive study of three different magnetic semiconductors, CrI3, CrBr3, and CrCl3, by incorporating both few-layer and bilayer samples in van der Waals tunnel junctions. We find that the interlayer magnetic ordering, exchange gap, magnetic anisotropy, and magnon excitations evolve systematically with changing halogen atom. By fitting to a spin wave theory that accounts for nearest-neighbor exchange interactions, we are able to further determine a simple spin Hamiltonian describing all three systems. These results extend the 2D magnetism platform to Ising, Heisenberg, and XY spin classes in a single material family. Using magneto-optical measurements, we additionally demonstrate that ferromagnetism can be stabilized down to monolayer in more isotropic CrBr3, with transition temperature still close to that of the bulk.