Correlated Charge Density Wave Insulators in Chirally Twisted Triple Bilayer Graphene.

Electrons residing in a flat-band system can play a vital role in triggering spectacular phenomenology due to relatively large interactions and spontaneous breaking of different degeneracies. In this work, we demonstrate chirally twisted triple bilayer graphene, a new moiré structure formed by three pieces of helically stacked Bernal bilayer graphene, as a highly tunable flat-band system. In addition to the correlated insulators showing at integer moiré fillings, commonly attributed to interaction induced symmetry broken isospin flavors in graphene, we observe abundant insulating states at half-integer moiré fillings, suggesting a longer-range interaction and the formation of charge density wave insulators which spontaneously break the moiré translation symmetry. With weak out-of-plane magnetic field applied, as observed half-integer filling states are enhanced and more quarter-integer filling states appear, pointing toward further quadrupling moiré unit cells. The insulating states at fractional fillings combined with Hartree-Fock calculations demonstrate the observation of a new type of correlated charge density wave insulators in graphene and points to a new accessible twist manner engineering correlated moiré electronics.

Magneto-Thermoelectric Transport in Graphene Quantum Dot with Strong Correlations.

Disorder at etched edges of graphene quantum dots (GQD) enables random all-to-all interactions between localized charges in partially filled Landau levels, providing a potential platform to realize the Sachdev-Ye-Kitaev (SYK) model. We use quantum Hall edge states in the graphene electrodes to measure electrical conductance and thermoelectric power across the GQD. In specific temperature ranges, we observe a suppression of electric conductance fluctuations and slowly decreasing thermoelectric power across the GQD with increasing temperature, consistent with recent theory for the SYK regime.

Anomalous Interlayer Exciton Diffusion in WS2/WSe2 Moiré Heterostructure.

Stacking van der Waals crystals allows for the on-demand creation of a periodic potential landscape to tailor the transport of quasiparticle excitations. We investigate the diffusion of photoexcited electron-hole pairs, or excitons, at the interface of WS2/WSe2 van der Waals heterostructure over a wide range of temperatures. We observe the appearance of distinct interlayer excitons for parallel and antiparallel stacking and track their diffusion through spatially and temporally resolved photoluminescence spectroscopy from 30 to 250 K. While the measured exciton diffusivity decreases with temperature, it surprisingly plateaus below 90 K. Our observations cannot be explained by classical models like hopping in the moiré potential. A combination of ab initio theory and molecular dynamics simulations suggests that low-energy phonons arising from the mismatched lattices of moiré heterostructures, also known as phasons, play a key role in describing and understanding this anomalous behavior of exciton diffusion. Our observations indicate that the moiré potential landscape is dynamic down to very low temperatures and that the phason modes can enable efficient transport of energy in the form of excitons.

Imaging tunable Luttinger liquid systems in van der Waals heterostructures.

One-dimensional (1D) interacting electrons are often described as a Luttinger liquid1-4 having properties that are intrinsically different from those of Fermi liquids in higher dimensions5,6. In materials systems, 1D electrons exhibit exotic quantum phenomena that can be tuned by both intra- and inter-1D-chain electronic interactions, but their experimental characterization can be challenging. Here we demonstrate that layer-stacking domain walls (DWs) in van der Waals heterostructures form a broadly tunable Luttinger liquid system, including both isolated and coupled arrays. We have imaged the evolution of DW Luttinger liquids under different interaction regimes tuned by electron density using scanning tunnelling microscopy. Single DWs at low carrier density are highly susceptible to Wigner crystallization consistent with a spin-incoherent Luttinger liquid, whereas at intermediate densities dimerized Wigner crystals form because of an enhanced magneto-elastic coupling. Periodic arrays of DWs exhibit an interplay between intra- and inter-chain interactions that gives rise to new quantum phases. At low electron densities, inter-chain interactions are dominant and induce a 2D electron crystal composed of phased-locked 1D Wigner crystal in a staggered configuration. Increased electron density causes intra-chain fluctuation potentials to dominate, leading to an electronic smectic liquid crystal phase in which electrons are ordered with algebraical correlation decay along the chain direction but disordered between chains. Our work shows that layer-stacking DWs in 2D heterostructures provides opportunities to explore Luttinger liquid physics.

Electrically tunable giant Nernst effect in two-dimensional van der Waals heterostructures.

The Nernst effect, a transverse thermoelectric phenomenon, has attracted significant attention for its potential in energy conversion, thermoelectrics and spintronics. However, achieving high performance and versatility at low temperatures remains elusive. Here we demonstrate a large and electrically tunable Nernst effect by combining the electrical properties of graphene with the semiconducting characteristics of indium selenide in a field-effect geometry. Our results establish a new platform for exploring and manipulating this thermoelectric effect, showcasing the first electrical tunability with an on/off ratio of 103. Moreover, photovoltage measurements reveal a stronger photo-Nernst signal in the graphene/indium selenide heterostructure compared with individual components. Remarkably, we observe a record-high Nernst coefficient of 66.4 µV K-1 T-1 at ultralow temperatures and low magnetic fields, an important step towards applications in quantum information and low-temperature emergent phenomena.

Wigner molecular crystals from multielectron moiré artificial atoms.

Semiconductor moiré superlattices provide a versatile platform to engineer quantum solids composed of artificial atoms on moiré sites. Previous studies have mostly focused on the simplest correlated quantum solid-the Fermi-Hubbard model-in which intra-atom interactions are simplified to a single onsite repulsion energy U. Here we report the experimental observation of Wigner molecular crystals emerging from multielectron artificial atoms in twisted bilayer tungsten disulfide moiré superlattices. Using scanning tunneling microscopy, we demonstrate that Wigner molecules appear in multielectron artificial atoms when Coulomb interactions dominate. The array of Wigner molecules observed in a moiré superlattice comprises a crystalline phase of electrons: the Wigner molecular crystal, which is shown to be highly tunable through mechanical strain, moiré period, and carrier charge type.

Selective and quasi-continuous switching of ferroelectric Chern insulator devices for neuromorphic computing.

Quantum materials exhibit dissipationless topological edge state transport with quantized Hall conductance, offering notable potential for fault-tolerant computing technologies. However, the development of topological edge state-based computing devices remains a challenge. Here we report the selective and quasi-continuous ferroelectric switching of topological Chern insulator devices, showcasing a proof-of-concept demonstration in noise-immune neuromorphic computing. We fabricate this ferroelectric Chern insulator device by encapsulating magic-angle twisted bilayer graphene with doubly aligned h-BN layers and observe the coexistence of the interfacial ferroelectricity and the topological Chern insulating states. The observed ferroelectricity exhibits an anisotropic dependence on the in-plane magnetic field. By tuning the amplitude of the gate voltage pulses, we achieve ferroelectric switching between any pair of Chern insulating states in the presence of a finite magnetic field, resulting in 1,280 ferroelectric states with distinguishable Hall resistance levels on a single device. Furthermore, we demonstrate deterministic switching between two arbitrary levels among the record-high number of ferroelectric states. This unique switching capability enables the implementation of a convolutional neural network resistant to external noise, utilizing the quantized Hall conductance levels of the Chern insulator device as weights. Our study provides a promising avenue towards the development of topological quantum neuromorphic computing, where functionality and performance can be drastically enhanced by topological quantum materials.

Sliding Memristor in Parallel-Stacked Hexagonal Boron Nitride.

Sliding ferroelectricity in 2D materials, arising from interlayer sliding-induced interlayer hybridization and charge redistribution at the van der Waals interface, offers a means to manipulate spontaneous polarization at the atomic scale through various methods such as stacking order, interfacial contact, and electric field. However, the practical application of extending 2D sliding ferroelectricity remains challenging due to the contentious mechanisms and the complex device structures required for ferroelectric switching. Here, a sliding memristor based on a graphene/parallel-stacked hexagonal boron nitride/graphene tunneling device, featuring a stable memristive hysteresis induced by interfacial polarizations and barrier height modulations, is presented. As the tunneling current density increases, the memristive window broadens, achieving an on/off ratio of ≈103 and 2 order decrease of the trigger current density, attributed to the interlayer migration of positively charged boron ions and the formation of conductive filaments, as supported by the theoretical calculations. The findings open a path for exploring the sliding memristor via a tunneling device and bridge the gap between sliding ferroelectricity and memory applications.

In situ via Contact to hBN-Encapsulated Air-Sensitive Atomically Thin Semiconductors.

Establishing reliable electrical contacts to atomically thin materials is a prerequisite for both fundamental studies and applications yet remains a challenge. In particular, the development of contact techniques for air-sensitive monolayers has lagged behind, despite their unique properties and significant potential for applications. Here, we present a robust method to create contacts to device layers encapsulated within hexagonal boron nitride (hBN). This method uses plasma etching and metal deposition to create 'vias' in the hBN with graphene forming an atomically thin etch-stop. The resulting partially fluorinated graphene (PFG) protects the underlying device layer from air-induced degradation and damage during metal deposition. PFG is resistive in-plane but maintains high out-of-plane conductivity. The work function of the PFG/metal contact is tunable through the degree of fluorination, offering opportunities for contact engineering. Using the in situ via technique, we achieve ambipolar contact to air-sensitive monolayer 2H-molybdenum ditelluride (MoTe2) with more than 1 order of magnitude improvement in on-current density compared to previous literature. The complete encapsulation provides high reproducibility and long-term stability. The technique can be extended to other air-sensitive materials as well as air-stable materials, offering highly competitive device performance.

Crossover between rigid and reconstructed moiré lattice in h-BN-encapsulated twisted bilayer WSe2 with different twist angles.

A moiré lattice in a twisted-bilayer transition metal dichalcogenide (tBL-TMD) exhibits a complex atomic reconstruction effect when its twist angle is less than a few degrees. The influence of the atomic reconstruction on material properties of the tBL-TMD has been of particular interest. In this study, we performed scanning transmission electron microscopy (STEM) imaging of a moiré lattice in h-BN-encapsulated twisted bilayer WSe2 with various twist angles. Atomic-resolution imaging of the moiré lattice revealed a reconstructed moiré lattice below a crossover twist angle of ∼4° and a rigid moiré lattice above this angle. Our findings indicate that h-BN encapsulation has a considerable influence on lattice reconstruction, as the crossover twist angle was larger in h-BN-encapsulated devices compared to non-encapsulated devices. We believe that this difference is due to the improved flatness and uniformity of the twisted bilayers with h-BN encapsulation. Our results provide a foundation for a deeper understanding of the lattice reconstruction in twisted TMD materials with h-BN encapsulation.

Berry curvature signatures in chiroptical excitonic transitions.

The topology of the electronic band structure of solids can be described by its Berry curvature distribution across the Brillouin zone. We theoretically introduce and experimentally demonstrate a general methodology based on the measurement of energy- and momentum-resolved optical transition rates, allowing to reveal signatures of Berry curvature texture in reciprocal space. By performing time- and angle-resolved photoemission spectroscopy of atomically thin WSe2 using polarization-modulated excitations, we demonstrate that excitons become an asset in extracting the quantum geometrical properties of solids. We also investigate the resilience of our measurement protocol against ultrafast scattering processes following direct chiroptical transitions.

Electric Dipole Coupling of a Bilayer Graphene Quantum Dot to a High-Impedance Microwave Resonator.

We implement circuit quantum electrodynamics (cQED) with quantum dots in bilayer graphene, a maturing material platform that can host long-lived spin and valley states. Our device combines a high-impedance (Zr ≈ 1 kΩ) superconducting microwave resonator with a double quantum dot electrostatically defined in a graphene-based van der Waals heterostructure. Electric dipole coupling between the subsystems allows the resonator to sense the electric susceptibility of the double quantum dot from which we reconstruct its charge stability diagram. We achieve sensitive and fast detection of the interdot transition with a signal-to-noise ratio of 3.5 within 1 µs integration time. The charge-photon interaction is quantified in the dispersive and resonant regimes by comparing the resonator response to input-output theory, yielding a coupling strength of g/2π = 49.7 MHz. Our results introduce cQED as a probe for quantum dots in van der Waals materials and indicate a path toward coherent charge-photon coupling with bilayer graphene quantum dots.

Multifunctional In-Memory Logics Based on a Dual-Gate Antiambipolar Transistor toward Non-von Neumann Computing Architecture.

In-memory computing may make it possible to realize non-von Neumann computing because the logic circuits are unified in the memory units. We investigated two types of in-memory logic operations, namely, two-input logic circuits and multifunctional artificial synapses. These were realized in a dual-gate antiambipolar transistor (AAT) with a ReS2/WSe2 heterojunction, in which polystyrene with a zinc phthalocyanine core (ZnPc-PS4) was incorporated as a memory layer. Here, reconfigurability is a key concept for both types of device operations and was achieved by merging the Λ-shaped transfer curve of the AAT and the nonvolatile memory effect of ZnPc-PS4. First, we achieved electrically reconfigurable two-input logic circuits. Versatile logic circuits such as AND, OR, NAND, NOR, and XOR circuits were demonstrated by taking advantage of the Λ-shaped transfer curve of the dual-gate AAT. Importantly, the nonvolatile memory function provided the electrical switching of the individual circuits between AND/OR, NAND/NOR, and XOR/NAND circuits with constant input signals. Second, the memory effect was applied to multifunctional artificial synapses. The inhibitory/excitatory and long-term potentiation/depression synaptic operations were electrically reconfigured simply by controlling one parameter (readout voltage), making three distinct responses possible even with the same presynaptic signals. These findings provide hints that may lead to the realization of new in-memory computing architectures beyond the current von Neumann computers.

Ultrafast high-endurance memory based on sliding ferroelectrics.

The persistence of voltage-switchable collective electronic phenomena down to the atomic scale has extensive implications for area- and energy-efficient electronics, especially in emerging nonvolatile memory technology. We investigate the performance of a ferroelectric field-effect transistor (FeFET) based on sliding ferroelectricity in bilayer boron nitride at room temperature. Sliding ferroelectricity represents a different form of atomically thin two-dimensional (2D) ferroelectrics, characterized by the switching of out-of-plane polarization through interlayer sliding motion. We examined the FeFET device employing monolayer graphene as the channel layer, which demonstrated ultrafast switching speeds on the nanosecond scale and high endurance exceeding 1011 switching cycles, comparable to state-of-the-art FeFET devices. These characteristics highlight the potential of 2D sliding ferroelectrics for inspiring next-generation nonvolatile memory technology.

Ultrafast Opto-Electronic and Thermal Tuning of Third-Harmonic Generation in a Graphene Field Effect Transistor.

Graphene is a unique platform for tunable opto-electronic applications thanks to its linear band dispersion, which allows electrical control of resonant light-matter interactions. Tuning the nonlinear optical response of graphene is possible both electrically and in an all-optical fashion, but each approach involves a trade-off between speed and modulation depth. Here, lattice temperature, electron doping, and all-optical tuning of third-harmonic generation are combined in a hexagonal boron nitride-encapsulated graphene opto-electronic device and demonstrate up to 85% modulation depth along with gate-tunable ultrafast dynamics. These results arise from the dynamic changes in the transient electronic temperature combined with Pauli blocking induced by the out-of-equilibrium chemical potential. The work provides a detailed description of the transient nonlinear optical and electronic response of graphene, which is crucial for the design of nanoscale and ultrafast optical modulators, detectors, and frequency converters.

Topology-Driven Coulomb Drag in van der Waals Heterostructure with Broken Inversion Symmetry.

As Coulomb drag near charge neutrality (CN) is driven by fluctuations or inhomogeneity in charge density, the topology should play an extremely important role. Interlinking Coulomb drag and topology could reveal how the system's nontrivial topology influences the electron-electron interactions at the quantum level. However, such an aspect is overlooked as most studies focus on symmetric drag systems without topology. To understand this topological aspect, we need to study Coulomb drag in an asymmetric system with a broken inversion symmetry and strong spin-orbit coupling (SOC). Here we experimentally demonstrate the energy-driven Coulomb drag in an asymmetric van der Waals heterostructure composed of black phosphorus and rhenium disulfide characterized by broken inversion symmetry. Temperature-dependent transport measurements near CN provide compelling evidence for the energy-driven Coulomb drag due to electron-hole coupling that is energetically favored in a broken-gap heterojunction, as confirmed by Hall coefficient sign reversal with temperature. Moreover, contrary to the symmetric devices, our results exhibit magnetic-field-free, i.e., topology-driven, Hall drag, revealing an intrinsic coupling between energy and charge modes. This is the manifestation of nonzero Berry curvature, akin to a magnetic field in momentum space, in a Rashba system, which arises from the SOC and broken inversion symmetry of the heterostructure.

Doping-control of excitons and magnetism in few-layer CrSBr.

Magnetism in two-dimensional materials reveals phenomena distinct from bulk magnetic crystals, with sensitivity to charge doping and electric fields in monolayer and bilayer van der Waals magnet CrI3. Within the class of layered magnets, semiconducting CrSBr stands out by featuring stability under ambient conditions, correlating excitons with magnetic order and thus providing strong magnon-exciton coupling, and exhibiting peculiar magneto-optics of exciton-polaritons. Here, we demonstrate that both exciton and magnetic transitions in bilayer and trilayer CrSBr are sensitive to voltage-controlled field-effect charging, exhibiting bound exciton-charge complexes and doping-induced metamagnetic transitions. Moreover, we demonstrate how these unique properties enable optical probes of local magnetic order, visualizing magnetic domains of competing phases across metamagnetic transitions induced by magnetic field or electrostatic doping. Our work identifies few-layer CrSBr as a rich platform for exploring collaborative effects of charge, optical excitations, and magnetism.

Quantum coherence and interference of a single moiré exciton in nano-fabricated twisted monolayer semiconductor heterobilayers.

The moiré potential serves as a periodic quantum confinement for optically generated excitons, creating spatially ordered zero-dimensional quantum systems. However, a broad emission spectrum resulting from inhomogeneity among moiré potentials hinders the investigation of their intrinsic properties. In this study, we demonstrated a method for the optical observation of quantum coherence and interference of a single moiré exciton in a twisted semiconducting heterobilayer beyond the diffraction limit of light. We observed a single and sharp photoluminescence peak from a single moiré exciton following nanofabrication. Our findings revealed the extended duration of quantum coherence in a single moiré exciton, persisting beyond 10 ps, and an accelerated decoherence process with increasing temperature and excitation power density. Moreover, quantum interference experiments revealed the coupling between moiré excitons in different moiré potential minima. The observed quantum coherence and interference of moiré exciton will facilitate potential applications of moiré quantum systems in quantum technologies.

Chern Insulator States with Tunable Chern Numbers in a Graphene Moiré Superlattice.

Moiré superlattices, constituted by two-dimensional materials, demonstrate a variety of strongly correlated and topological phenomena including correlated insulators, superconductivity, and integer/fractional Chern insulators. In the realm of topological nontrivial Chern insulators within specific moiré superlattices, previous studies usually observe a single Chern number at a given filling factor in a device. Here we present the observation of gate-tunable Chern numbers within the Chern insulator state of an ABC-stacked trilayer graphene/hexagonal boron nitride moiré superlattice device. Near quarter filling, the moiré superlattice exhibits spontaneous valley polarization and distinct ferromagnetism associated with the Chern insulator states over a range of the displacement field. Surprisingly we find a transition of the Chern number from C = 3 to 4 as the displacement field is increased. Our observation of gate-tunable correlated Chern insulators suggests new ways to control and manipulate topological states in a moiré superlattice device.

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.