Linear resistivity at van Hove singularities in twisted bilayer WSe2.

Different mechanisms driving a linear temperature dependence of the resistivity ρ ∼ T at van Hove singularities (VHSs) or metal-insulator transitions when doping a Mott insulator are being debated intensively with competing theoretical proposals. We experimentally investigate this using the exceptional tunability of twisted bilayer (TB) WSe2 by tracking the parameter regions where linear-in-T resistivity is found in dependency of displacement fields, filling, and magnetic fields. We find that even when the VHSs are tuned rather far away from the half-filling point and the Mott insulating transition is absent, the T-linear resistivity persists at the VHSs. When doping away from the VHSs, the T-linear behavior quickly transitions into a Fermi liquid behavior with a T2 relation. No apparent dependency of the linear-in-T resistivity, besides a rather strong change of prefactor, is found when applying displacement fields as long as the filling is tuned to the VHSs, including D ∼ 0.28 V/nm where a high-order VHS is expected. Intriguingly, such non-Fermi liquid linear-in-T resistivity persists even when magnetic fields break the spin-degeneracy of the VHSs at which point two linear in T regions emerge, for each of the split VHSs separately. This points to a mechanism of enhanced scattering at generic VHSs rather than only at high-order VHSs or by a quantum critical point during a Mott transition. Our findings provide insights into the many-body consequences arising out of VHSs, especially the non-Fermi liquid behavior found in moiré materials.

Gate-Tunable Multiband van der Waals Photodetector and Polarization Sensor.

A single photodetector with tunable detection wavelengths and polarization sensitivity can potentially be harnessed for diverse optical applications ranging from imaging and sensing to telecommunications. Such a device will require the combination of multiple material systems with different structures, band gaps, and photoelectrical responses, which is extremely difficult to engineer using traditional epitaxial films. Here, we develop a multifunctional and high-performance photosensor using all van der Waals materials. The device features a gate-tunable spectral response that is switchable between near-infrared/visible and short-/midwave infrared, as well as broad-band operation, at room temperature. The linear polarization sensitivity in the telecommunication O-band can also be directly modulated between horizontal, vertical, and nonpolarizing modes. These effects originate from the balance of photocurrent generation in two of the active layers that can be manipulated by an electric field. The photodetector features high detectivity (>109 cmHz1/2W-1) together with fast operation speed (∼1 MHz) and can be further exploited for dual visible and infrared imaging.

Programmable nanowrinkle-induced room-temperature exciton localization in monolayer WSe2.

Localized states in two-dimensional (2D) transition metal dichalcogenides (TMDCs) have been the subject of intense study, driven by potential applications in quantum information science. Despite the rapidly growing knowledge surrounding these emitters, their microscopic nature is still not fully understood, limiting their production and application. Motivated by this challenge, and by recent theoretical and experimental evidence showing that nanowrinkles generate strain-localized room-temperature emitters, we demonstrate a method to intentionally induce wrinkles with collections of stressors, showing that long-range wrinkle direction and position are controllable with patterned array design. Nano-photoluminescence (nano-PL) imaging combined with detailed strain modeling based on measured wrinkle topography establishes a correlation between wrinkle properties, particularly shear strain, and localized exciton emission. Beyond the array-induced wrinkles, nano-PL spatial maps further reveal that the strain environment around individual stressors is heterogeneous due to the presence of fine wrinkles that are less deterministic. At cryogenic temperatures, antibunched emission is observed, confirming that the nanocone-induced strain is sufficiently large for the formation of quantum emitters. At 300 K, detailed nanoscale hyperspectral images uncover a wide range of low-energy emission peaks originating from the fine wrinkles, and show that the states can be tightly confined to regions <10 nm, even in ambient conditions. These results establish a promising potential route towards realizing room temperature quantum emission in 2D TMDC systems.

Transport Study of Charge-Carrier Scattering in Monolayer WSe_{2}.

Employing flux-grown single crystal WSe_{2}, we report charge-carrier scattering behaviors measured in h-BN encapsulated monolayer field effect transistors. We observe a nonmonotonic change of transport mobility as a function of hole density in the degenerately doped sample, which can be explained by energy dependent scattering amplitude of strong defects calculated using the T-matrix approximation. Utilizing long mean-free path (>500 nm), we also demonstrate the high quality of our electronic devices by showing quantized conductance steps from an electrostatically defined quantum point contact, showing the potential for creating ultrahigh quality quantum optoelectronic devices based on atomically thin semiconductors.

Two-Step Flux Synthesis of Ultrapure Transition-Metal Dichalcogenides.

Two-dimensional transition-metal dichalcogenides (TMDs) have attracted tremendous interest due to the unusual electronic and optoelectronic properties of isolated monolayers and the ability to assemble diverse monolayers into complex heterostructures. To understand the intrinsic properties of TMDs and fully realize their potential in applications and fundamental studies, high-purity materials are required. Here, we describe the synthesis of TMD crystals using a two-step flux growth method that eliminates a major potential source of contamination. Detailed characterization of TMDs grown by this two-step method reveals charged and isovalent defects with densities an order of magnitude lower than those in TMDs grown by a single-step flux technique. For WSe2, we show that increasing the Se/W ratio during growth reduces point defect density, with crystals grown at 100:1 ratio achieving charged and isovalent defect densities below 1010 and 1011 cm-2, respectively. Initial temperature-dependent electrical transport measurements of monolayer WSe2 yield room-temperature hole mobility above 840 cm2/(V s) and low-temperature disorder-limited mobility above 44,000 cm2/(V s). Electrical transport measurements of graphene-WSe2 heterostructures fabricated from the two-step flux grown WSe2 also show superior performance: higher graphene mobility, lower charged impurity density, and well-resolved integer quantum Hall states. Finally, we demonstrate that the two-step flux technique can be used to synthesize other TMDs with similar defect densities, including semiconducting 2H-MoSe2 and 2H-MoTe2 and semimetallic Td-WTe2 and 1T'-MoTe2.

Coupled ferroelectricity and superconductivity in bilayer Td-MoTe2.

Achieving electrostatic control of quantum phases is at the frontier of condensed matter research. Recent investigations have revealed superconductivity tunable by electrostatic doping in twisted graphene heterostructures and in two-dimensional semimetals such as WTe2 (refs. 1-5). Some of these systems have a polar crystal structure that gives rise to ferroelectricity, in which the interlayer polarization exhibits bistability driven by external electric fields6-8. Here we show that bilayer Td-MoTe2 simultaneously exhibits ferroelectric switching and superconductivity. Notably, a field-driven, first-order superconductor-to-normal transition is observed at its ferroelectric transition. Bilayer Td-MoTe2 also has a maximum in its superconducting transition temperature (Tc) as a function of carrier density and temperature, allowing independent control of the superconducting state as a function of both doping and polarization. We find that the maximum Tc is concomitant with compensated electron and hole carrier densities and vanishes when one of the Fermi pockets disappears with doping. We argue that this unusual polarization-sensitive two-dimensional superconductor is driven by an interband pairing interaction associated with nearly nested electron and hole Fermi pockets.

High-Performance Mid-IR to Deep-UV van der Waals Photodetectors Capable of Local Spectroscopy at Room Temperature.

The ability to perform broadband optical spectroscopy with subdiffraction-limit resolution is highly sought-after for a wide range of critical applications. However, sophisticated near-field techniques are currently required to achieve this goal. We bypass this challenge by demonstrating an extremely broadband photodetector based on a two-dimensional (2D) van der Waals heterostructure that is sensitive to light across over a decade in energy from the mid-infrared (MIR) to deep-ultraviolet (DUV) at room temperature. The devices feature high detectivity (>109 cm Hz1/2 W-1) together with high bandwidth (2.1 MHz). The active area can be further miniaturized to submicron dimensions, far below the diffraction limit for the longest detectable wavelength of 4.1 µm, enabling such devices for facile measurements of local optical properties on atomic-layer-thickness samples placed in close proximity. This work can lead to the development of low-cost and high-throughput photosensors for hyperspectral imaging at the nanoscale.

Dissipation-enabled hydrodynamic conductivity in a tunable bandgap semiconductor.

Electronic transport in the regime where carrier-carrier collisions are the dominant scattering mechanism has taken on new relevance with the advent of ultraclean two-dimensional materials. Here, we present a combined theoretical and experimental study of ambipolar hydrodynamic transport in bilayer graphene demonstrating that the conductivity is given by the sum of two Drude-like terms that describe relative motion between electrons and holes, and the collective motion of the electron-hole plasma. As predicted, the measured conductivity of gapless, charge-neutral bilayer graphene is sample- and temperature-independent over a wide range. Away from neutrality, the electron-hole conductivity collapses to a single curve, and a set of just four fitting parameters provides quantitative agreement between theory and experiment at all densities, temperatures, and gaps measured. This work validates recent theories for dissipation-enabled hydrodynamic conductivity and creates a link between semiconductor physics and the emerging field of viscous electronics.

Manipulation of Exciton Dynamics in Single-Layer WSe2 Using a Toroidal Dielectric Metasurface.

Recent advances in emerging atomically thin transition metal dichalcogenide semiconductors with strong light-matter interactions and tunable optical properties provide novel approaches for realizing new material functionalities. Coupling two-dimensional semiconductors with all-dielectric resonant nanostructures represents an especially attractive opportunity for manipulating optical properties in both the near-field and far-field regimes. Here, by integrating single-layer WSe2 and titanium oxide (TiO2) dielectric metasurfaces with toroidal resonances, we realized robust exciton emission enhancement over 1 order of magnitude at both room and low temperatures. Furthermore, we could control exciton dynamics and annihilation by using temperature to tailor the spectral overlap of excitonic and toroidal resonances, allowing us to selectively enhance the Purcell effect. Our results provide rich physical insight into the strong light-matter interactions in single-layer TMDs coupled with toroidal dielectric metasurfaces, with important implications for optoelectronics and photonics applications.

Quantum criticality in twisted transition metal dichalcogenides.

Near the boundary between ordered and disordered quantum phases, several experiments have demonstrated metallic behaviour that defies the Landau Fermi paradigm1-5. In moiré heterostructures, gate-tuneable insulating phases driven by electronic correlations have been recently discovered6-23. Here, we use transport measurements to characterize metal-insulator transitions (MITs) in twisted WSe2 near half filling of the first moiré subband. We find that the MIT as a function of both density and displacement field is continuous. At the metal-insulator boundary, the resistivity displays strange metal behaviour at low temperatures, with dissipation comparable to that at the Planckian limit. Further into the metallic phase, Fermi liquid behaviour is recovered at low temperature, and this evolves into a quantum critical fan at intermediate temperatures, before eventually reaching an anomalous saturated regime near room temperature. An analysis of the residual resistivity indicates the presence of strong quantum fluctuations in the insulating phase. These results establish twisted WSe2 as a new platform to study doping and bandwidth-controlled metal-insulator quantum phase transitions on the triangular lattice.

Long-Lived Phonon Polaritons in Hyperbolic Materials.

Natural hyperbolic materials with dielectric permittivities of opposite signs along different principal axes can confine long-wavelength electromagnetic waves down to the nanoscale, well below the diffraction limit. Confined electromagnetic waves coupled to phonons in hyperbolic dielectrics including hexagonal boron nitride (hBN) and α-MoO3 are referred to as hyperbolic phonon polaritons (HPPs). HPP dissipation at ambient conditions is substantial, and its fundamental limits remain unexplored. Here, we exploit cryogenic nanoinfrared imaging to investigate propagating HPPs in isotopically pure hBN and naturally abundant α-MoO3 crystals. Close to liquid-nitrogen temperatures, losses for HPPs in isotopic hBN drop significantly, resulting in propagation lengths in excess of 8 µm, with lifetimes exceeding 5 ps, thereby surpassing prior reports on such highly confined polaritonic modes. Our nanoscale, temperature-dependent imaging reveals the relevance of acoustic phonons in HPP damping and will be instrumental in mitigating such losses for miniaturized mid-infrared technologies operating at liquid-nitrogen temperatures.

Enhanced Superconductivity in Monolayer Td-MoTe2.

Crystalline two-dimensional (2D) superconductors (SCs) with low carrier density are an exciting new class of materials in which electrostatic gating can tune superconductivity, electronic interactions play a prominent role, and electrical transport properties may directly reflect the topology of the Fermi surface. Here, we report the dramatic enhancement of superconductivity with decreasing thickness in semimetallic Td-MoTe2, with critical temperature (Tc) increasing up to 7.6 K for monolayers, a 60-fold increase with respect to the bulk Tc. We show that monolayers possess a similar electronic structure and density of states (DOS) as the bulk, implying that electronic interactions play a strong role in the enhanced superconductivity. Reflecting the low carrier density, the critical temperature, magnetic field, and current density are all tunable by an applied gate voltage. The response to high in-plane magnetic fields is distinct from that of other 2D SCs and reflects the canted spin texture of the electron pockets.

Tunable Exciton-Optomechanical Coupling in Suspended Monolayer MoSe2.

The strong excitonic effect in monolayer transition metal dichalcogenide (TMD) semiconductors has enabled many fascinating light-matter interaction phenomena. Examples include strongly coupled exciton-polaritons and nearly perfect atomic monolayer mirrors. The strong light-matter interaction also opens the door for dynamical control of mechanical motion through the exciton resonance of monolayer TMDs. Here, we report the observation of exciton-optomechanical coupling in a suspended monolayer MoSe2 mechanical resonator. By moderate optical pumping near the MoSe2 exciton resonance, we have observed optical damping and antidamping of mechanical vibrations as well as the optical spring effect. The exciton-optomechanical coupling strength is also gate-tunable. Our observations can be understood in a model based on photothermal backaction and gate-induced mirror symmetry breaking in the device structure. The observation of gate-tunable exciton-optomechanical coupling in a monolayer semiconductor may find applications in nanoelectromechanical systems (NEMS) and in exciton-optomechanics.

Intrinsic donor-bound excitons in ultraclean monolayer semiconductors.

The monolayer transition metal dichalcogenides are an emergent semiconductor platform exhibiting rich excitonic physics with coupled spin-valley degree of freedom and optical addressability. Here, we report a new series of low energy excitonic emission lines in the photoluminescence spectrum of ultraclean monolayer WSe2. These excitonic satellites are composed of three major peaks with energy separations matching known phonons, and appear only with electron doping. They possess homogenous spatial and spectral distribution, strong power saturation, and anomalously long population (>6 µs) and polarization lifetimes (>100 ns). Resonant excitation of the free inter- and intravalley bright trions leads to opposite optical orientation of the satellites, while excitation of the free dark trion resonance suppresses the satellites' photoluminescence. Defect-controlled crystal synthesis and scanning tunneling microscopy measurements provide corroboration that these features are dark excitons bound to dilute donors, along with associated phonon replicas. Our work opens opportunities to engineer homogenous single emitters and explore collective quantum optical phenomena using intrinsic donor-bound excitons in ultraclean 2D semiconductors.

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.

Imaging strain-localized excitons in nanoscale bubbles of monolayer WSe2 at room temperature.

In monolayer transition-metal dichalcogenides, localized strain can be used to design nanoarrays of single photon sources. Despite strong empirical correlation, the nanoscale interplay between excitons and local crystalline structure that gives rise to these quantum emitters is poorly understood. Here, we combine room-temperature nano-optical imaging and spectroscopic analysis of excitons in nanobubbles of monolayer WSe2 with atomistic models to study how strain induces nanoscale confinement potentials and localized exciton states. The imaging of nanobubbles in monolayers with low defect concentrations reveals localized excitons on length scales of around 10 nm at multiple sites around the periphery of individual nanobubbles, in stark contrast to predictions of continuum models of strain. These results agree with theoretical confinement potentials atomistically derived from the measured topographies of nanobubbles. Our results provide experimental and theoretical insights into strain-induced exciton localization on length scales commensurate with exciton size, realizing key nanoscale structure-property information on quantum emitters in monolayer WSe2.

Odd- and even-denominator fractional quantum Hall states in monolayer WSe2.

Monolayer semiconducting transition-metal dichalcogenides (TMDs) represent a unique class of two-dimensional (2D) electron systems. Their atomically thin structure facilitates gate tunability just like graphene does, but unlike graphene, TMDs have the advantage of a sizable band gap and strong spin-orbit coupling. Measurements under large magnetic fields have revealed an unusual Landau level (LL) structure1-3, distinct from other 2D electron systems. However, owing to the limited sample quality and poor electrical contact, probing the lowest LLs has been challenging, and observation of electron correlations within the fractionally filled LL regime has not been possible. Here, through bulk electronic compressibility measurements, we investigate the LL structure of monolayer WSe2 in the extreme quantum limit, and observe fractional quantum Hall states in the lowest three LLs. The odd-denominator fractional quantum Hall sequences demonstrate a systematic evolution with the LL orbital index, consistent with generic theoretical expectations. In addition, we observe an even-denominator state in the second LL that is expected to host non-Abelian statistics. Our results suggest that the 2D semiconductors can provide an experimental platform that closely resembles idealized theoretical models in the quantum Hall regime.

Correlated electronic phases in twisted bilayer transition metal dichalcogenides.

In narrow electron bands in which the Coulomb interaction energy becomes comparable to the bandwidth, interactions can drive new quantum phases. Such flat bands in twisted graphene-based systems result in correlated insulator, superconducting and topological states. Here we report evidence of low-energy flat bands in twisted bilayer WSe2, with signatures of collective phases observed over twist angles that range from 4 to 5.1°. At half-band filling, a correlated insulator appeared that is tunable with both twist angle and displacement field. At a 5.1° twist, zero-resistance pockets were observed on doping away from half filling at temperatures below 3 K, which indicates a possible transition to a superconducting state. The observation of tunable collective phases in a simple band, which hosts only two holes per unit cell at full filling, establishes twisted bilayer transition metal dichalcogenides as an ideal platform to study correlated physics in two dimensions on a triangular lattice.

Direct Measurement of the Radiative Pattern of Bright and Dark Excitons and Exciton Complexes in Encapsulated Tungsten Diselenide.

The optical properties of particularly the tungsten-based transition-metal dichalcogenides are strongly influenced by the presence of dark excitons. Recently, theoretical predictions as well as indirect experimental insights have shown that two different dark excitons exist within the light cone. While one is completely dark, the other one is only dipole forbidden out-of-plane, hence referred to as grey exciton. Here, we present angle-resolved spectroscopic data of a high-quality hexagonal-BN-encapsulated WSe2 monolayer with which we directly obtain the radiation pattern of this grey exciton that deviates from that of the bright exciton and other exciton complexes obtained at cryogenic temperatures.

Near-Unity Light Absorption in a Monolayer WS2 Van der Waals Heterostructure Cavity.

Excitons in monolayer transition-metal-dichalcogenides (TMDs) dominate their optical response and exhibit strong light-matter interactions with lifetime-limited emission. While various approaches have been applied to enhance light-exciton interactions in TMDs, the achieved strength have been far below unity, and a complete picture of its underlying physical mechanisms and fundamental limits has not been provided. Here, we introduce a TMD-based van der Waals heterostructure cavity that provides near-unity excitonic absorption, and emission of excitonic complexes that are observed at ultralow excitation powers. Our results are in full agreement with a quantum theoretical framework introduced to describe the light-exciton-cavity interaction. We find that the subtle interplay between the radiative, nonradiative and dephasing decay rates plays a crucial role, and unveil a universal absorption law for excitons in 2D systems. This enhanced light-exciton interaction provides a platform for studying excitonic phase-transitions and quantum nonlinearities and enables new possibilities for 2D semiconductor-based optoelectronic devices.