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.

Maximized electron interactions at the magic angle in twisted bilayer graphene.

The electronic properties of heterostructures of atomically thin van der Waals crystals can be modified substantially by moiré superlattice potentials from an interlayer twist between crystals1,2. Moiré tuning of the band structure has led to the recent discovery of superconductivity3,4 and correlated insulating phases5 in twisted bilayer graphene (TBG) near the 'magic angle' of twist of about 1.1 degrees, with a phase diagram reminiscent of high-transition-temperature superconductors. Here we directly map the atomic-scale structural and electronic properties of TBG near the magic angle using scanning tunnelling microscopy and spectroscopy. We observe two distinct van Hove singularities (VHSs) in the local density of states around the magic angle, with an energy separation of 57 millielectronvolts that drops to 40 millielectronvolts with high electron/hole doping. Unexpectedly, the VHS energy separation continues to decrease with decreasing twist angle, with a lowest value of 7 to 13 millielectronvolts at a magic angle of 0.79 degrees. More crucial to the correlated behaviour of this material, we find that at the magic angle, the ratio of the Coulomb interaction to the bandwidth of each individual VHS (U/t) is maximized, which is optimal for electronic Cooper pairing mechanisms. When doped near the half-moiré-band filling, a correlation-induced gap splits the conduction VHS with a maximum size of 6.5 millielectronvolts at 1.15 degrees, dropping to 4 millielectronvolts at 0.79 degrees. We capture the doping-dependent and angle-dependent spectroscopy results using a Hartree-Fock model, which allows us to extract the on-site and nearest-neighbour Coulomb interactions. This analysis yields a U/t of order unity indicating that magic-angle TBG is moderately correlated. In addition, scanning tunnelling spectroscopy maps reveal an energy- and doping-dependent three-fold rotational-symmetry breaking of the local density of states in TBG, with the strongest symmetry breaking near the Fermi level and further enhanced when doped to the correlated gap regime. This indicates the presence of a strong electronic nematic susceptibility or even nematic order in TBG in regions of the phase diagram where superconductivity is observed.

Tip Growth of Quasi-Metallic Bilayer Graphene Nanoribbons with Armchair Chirality.

Graphene nanoribbons (GNRs), quasi one-dimensional (1D) narrow strips of graphene, have shown promise for high-performance nanoelectronics due to their exceptionally high carrier mobility and structurally tunable bandgaps. However, producing chirality-uniform GNRs on insulating substrates remains a big challenge. Here, we report the successful growth of bilayer GNRs with predominantly armchair chirality and ultranarrow widths (<5 nm) on insulating hexagonal boron nitride (h-BN) substrates using chemical vapor deposition (CVD). The growth of GNRs is catalyzed by transition metal nanoparticles, including Fe, Co, and Ni, through a unique tip-growth mechanism. Notably, GNRs catalyzed by Ni exhibit a high purity (97.3%) of armchair chirality. Electron transport measurements indicate that the ultrathin bilayer armchair GNRs exhibit quasi-metallic behavior. This quasi-metallicity is further supported by density functional theory (DFT) calculations, which reveal a significantly reduced bandgap in bilayer armchair GNRs. The chirality-specific GNRs reported here offer promising advancements for the application of graphene in nanoelectronics.

Moiréless correlations in ABCA graphene.

Atomically thin van der Waals materials stacked with an interlayer twist have proven to be an excellent platform toward achieving gate-tunable correlated phenomena linked to the formation of flat electronic bands. In this work we demonstrate the formation of emergent correlated phases in multilayer rhombohedral graphene--a simple material that also exhibits a flat electronic band edge but without the need of having a moiré superlattice induced by twisted van der Waals layers. We show that two layers of bilayer graphene that are twisted by an arbitrary tiny angle host large (micrometer-scale) regions of uniform rhombohedral four-layer (ABCA) graphene that can be independently studied. Scanning tunneling spectroscopy reveals that ABCA graphene hosts an unprecedentedly sharp van Hove singularity of 3-5-meV half-width. We demonstrate that when this van Hove singularity straddles the Fermi level, a correlated many-body gap emerges with peak-to-peak value of 9.5 meV at charge neutrality. Mean-field theoretical calculations for model with short-ranged interactions indicate that two primary candidates for the appearance of this broken symmetry state are a charge-transfer excitonic insulator and a ferrimagnet. Finally, we show that ABCA graphene hosts surface topological helical edge states at natural interfaces with ABAB graphene which can be turned on and off with gate voltage, implying that small-angle twisted double-bilayer graphene is an ideal programmable topological quantum material.

Switching the Moiré Lattice Models in the Twisted Bilayer WSe2 by Strain or Pressure.

Moiré superlattices of twisted van der Waals heterostructures provide a promising and tunable platform for simulating correlated two-dimensional physical models. In twisted bilayer transition-metal dichalcogenides with twist angles close to 0°, the Γ and K valley moiré bands are described by the honeycomb and the triangular effective lattice models, respectively, with distinct physics. Using large-scale first-principles calculations, we show that in-plane biaxial strain and out-of-plane pressure provide effective knobs for switching the moiré lattice models that emerged at the band edges in twisted bilayer WSe2 by shifting the energy positions of the Γ and K valley minibands. The shifting mechanism originates from the differences in the orbital characters of the Γ and K valley states and their responses to strain and pressure. The critical strain and pressure for switching the Γ/K valleys are 2.11% and 2.175 GPa, respectively.

Ultrafast Spin Dynamics and Photoinduced Insulator-to-Metal Transition in α-RuCl3.

Laser-induced ultrafast demagnetization is a phenomenon of utmost interest and attracts significant attention because it enables potential applications in ultrafast optoelectronics and spintronics. As a spin-orbit coupling assisted magnetic insulator, α-RuCl3 provides an attractive platform to explore the physics of electronic correlations and unconventional magnetism. Using time-dependent density functional theory, we explore the ultrafast laser-induced dynamics of the electronic and magnetic structures in α-RuCl3. Our study unveils that laser pulses can introduce ultrafast demagnetizations, accompanied by an out-of-equilibrium insulator-to-metal transition in a few tens of femtoseconds. The spin response significantly depends on the laser wavelength and polarization on account of the electron correlations, band renormalizations, and charge redistributions. These findings provide physical insights into the coupling between the electronic and magnetic degrees of freedom in α-RuCl3 and shed light on suppressing the long-range magnetic orders and reaching a proximate spin liquid phase for two-dimensional magnets on an ultrafast time scale.

Moiré enhanced charge density wave state in twisted 1T-TiTe2/1T-TiSe2 heterostructures.

Nanoscale periodic moiré patterns, for example those formed at the interface of a twisted bilayer of two-dimensional materials, provide opportunities for engineering the electronic properties of van der Waals heterostructures1-11. In this work, we synthesized the epitaxial heterostructure of 1T-TiTe2/1T-TiSe2 with various twist angles using molecular beam epitaxy and investigated the moiré pattern induced/enhanced charge density wave (CDW) states with scanning tunnelling microscopy. When the twist angle is near zero degrees, 2 × 2 CDW domains are formed in 1T-TiTe2, separated by 1 × 1 normal state domains, and trapped in the moiré pattern. The formation of the moiré-trapped CDW state is ascribed to the local strain variation due to atomic reconstruction. Furthermore, this CDW state persists at room temperature, suggesting its potential for future CDW-based applications. Such moiré-trapped CDW patterns were not observed at larger twist angles. Our study paves the way for constructing metallic twist van der Waals bilayers and tuning many-body effects via moiré engineering.

Giant Correlated Gap and Possible Room-Temperature Correlated States in Twisted Bilayer MoS_{2}.

Moiré superlattices have emerged as an exciting condensed-matter quantum simulator for exploring the exotic physics of strong electronic correlations. Notable progress has been witnessed, but such correlated states are achievable usually at low temperatures. Here, we report evidence of possible room-temperature correlated electronic states and layer-hybridized SU(4) model simulator in AB-stacked MoS_{2} homobilayer moiré superlattices. Correlated insulating states at moiré band filling factors v=1, 2, 3 are unambiguously established in twisted bilayer MoS_{2}. Remarkably, the correlated electronic state at v=1 shows a giant correlated gap of ∼126 meV and may persist up to a record-high critical temperature over 285 K. The realization of a possible room-temperature correlated state with a large correlated gap in twisted bilayer MoS_{2} can be understood as the cooperation effects of the stacking-specific atomic reconstruction and the resonantly enhanced interlayer hybridization, which largely amplify the moiré superlattice effects on electronic correlations. Furthermore, extreme large nonlinear Hall responses up to room temperature are uncovered near correlated electronic states, demonstrating the quantum geometry of moiré flat conduction band.

Engineering Three-Dimensional Moiré Flat Bands.

Twisting two adjacent layers of van der Waals materials with respect to each other can lead to flat two-dimensional electronic bands which enables a wealth of physical phenomena. Here, we generalize this concept of so-called moiré flat bands to engineer flat bands in all three spatial dimensions controlled by the twist angle. The basic concept is to stack the material such that the large spatial moiré interference patterns are spatially shifted from one twisted layer to the next. We exemplify the general concept by considering graphitic systems, boron nitride, and WSe2, but the approach is applicable to any two-dimensional van der Waals material. For hexagonal boron nitride, we develop an ab initio fitted tight binding model that captures the corresponding three-dimensional low-energy electronic structure. We outline that interesting three-dimensional correlated phases of matter can be induced and controlled following this route, including quantum magnets and unconventional superconducting states.

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.

Higher-Order Band Topology in Twisted Moiré Superlattice.

The two-dimensional (2D) twisted bilayer materials with van der Waals coupling have ignited great research interests, paving a new way to explore the emergent quantum phenomena by twist degree of freedom. Generally, with the decreasing of twist angle, the enhanced interlayer coupling will gradually flatten the low-energy bands and isolate them by two high-energy gaps at zero and full filling, respectively. Although the correlation and topological physics in the low-energy flat bands have been intensively studied, little information is available for these two emerging gaps. In this Letter, we predict a 2D second-order topological insulator (SOTI) for twisted bilayer graphene and twisted bilayer boron nitride in both zero and full filling gaps. Employing a tight-binding Hamiltonian based on first-principles calculations, three unique fingerprints of 2D SOTI are identified, that is, nonzero bulk topological index, gapped topological edge state, and in-gap topological corner state. Most remarkably, the 2D SOTI exists in a wide range of commensurate twist angles, which is robust to microscopic structure disorder and twist center, greatly facilitating the possible experimental measurement. Our results not only extend the higher-order band topology to massless and massive twisted moiré superlattice, but also demonstrate the importance of high-energy bands for fully understanding the nontrivial electronics.

Charge-Transfer Plasmon Polaritons at Graphene/α-RuCl3 Interfaces.

Nanoscale charge control is a key enabling technology in plasmonics, electronic band structure engineering, and the topology of two-dimensional materials. By exploiting the large electron affinity of α-RuCl3, we are able to visualize and quantify massive charge transfer at graphene/α-RuCl3 interfaces through generation of charge-transfer plasmon polaritons (CPPs). We performed nanoimaging experiments on graphene/α-RuCl3 at both ambient and cryogenic temperatures and discovered robust plasmonic features in otherwise ungated and undoped structures. The CPP wavelength evaluated through several distinct imaging modalities offers a high-fidelity measure of the Fermi energy of the graphene layer: EF = 0.6 eV (n = 2.7 × 1013 cm-2). Our first-principles calculations link the plasmonic response to the work function difference between graphene and α-RuCl3 giving rise to CPPs. Our results provide a novel general strategy for generating nanometer-scale plasmonic interfaces without resorting to external contacts or chemical doping.

Multiflat Bands and Strong Correlations in Twisted Bilayer Boron Nitride: Doping-Induced Correlated Insulator and Superconductor.

Two-dimensional materials, obtained by van der Waals stacking of layers, are fascinating objects of contemporary condensed matter research, exhibiting a variety of new physics. Inspired by the breakthroughs of twisted bilayer graphene (TBG), we demonstrate that twisted bilayer boron nitride (TBBN) is an even more exciting novel system that turns out to be an excellent platform to realize new correlated phases and phenomena; exploration of its electronic properties shows that in contrast to TBG in TBBN multiple families of 2,4, and 6-fold degenerate flat bands emerge without the need to fine tune close to a "magic angle", resulting in dramatic and tunable changes in optical properties and exciton physics, and providing an additional platform to study strong correlations. Upon doping, unforeseen new correlated phases of matter (insulating and superconducting) emerge. TBBN could thus provide a promising experimental platform, insensitive to small deviations in the twist angle, to study novel exciton condensate and spatial confinement physics, and correlations in two dimensions.

Instantaneous band gap collapse in photoexcited monoclinic VO2 due to photocarrier doping.

Using femtosecond time-resolved photoelectron spectroscopy we demonstrate that photoexcitation transforms monoclinic VO2 quasi-instantaneously into a metal. Thereby, we exclude an 80 fs structural bottleneck for the photoinduced electronic phase transition of VO2. First-principles many-body perturbation theory calculations reveal a high sensitivity of the VO2 band gap to variations of the dynamically screened Coulomb interaction, supporting a fully electronically driven isostructural insulator-to-metal transition. We thus conclude that the ultrafast band structure renormalization is caused by photoexcitation of carriers from localized V 3d valence states, strongly changing the screening before significant hot-carrier relaxation or ionic motion has occurred.

Coupled Dirac fermions and neutrino-like oscillations in twisted bilayer graphene.

The low-energy quasiparticles in graphene can be described by a Dirac-Weyl Hamiltonian for massless fermions, hence graphene has been proposed to be an effective medium to study exotic phenomena originally predicted for relativistic particle physics, such as Klein tunneling and Zitterbewegung. In this work, we show that another important particle-physics phenomenon, the neutrino oscillation, can be studied and observed in a particular graphene system, namely, twisted bilayer graphene. It has been found that graphene layers grown epitaxially on SiC or by the chemical vapor deposition method on metal substrates display a stacking pattern with adjacent layers rotated by an angle with respect to each other. The quasiparticle states in two distinct graphene layers act as neutrinos with two flavors, and the interlayer interaction between them induces an appreciable coupling between these two "flavors" of massless fermions, leading to neutrino-like oscillations. In addition, our calculation shows that anisotropic transport properties manifest in a specific energy window, which is accessible experimentally in twisted bilayer graphene. Combining two graphene layers enables us to probe the rich physics involving multiple interacting Dirac fermions.

In Situ Growth of MoS2 Onto Co-Based MOF Derivatives Toward High-Efficiency Quantum Dot-Sensitized Solar Cells.

Quantum dot sensitized solar cells (QDSCs) represent a promising third-generation photovoltaic technology, boasting a high theoretical efficiency of 44% and cost efficiency. However, their practical efficiency is constrained by reduced photovoltage (Voc) and fill factor (FF). One primary reason is the inefficient charge transfer and elevated recombination rates at the counter electrode (CE). In this work, a novel CE composed of a titanium mesh loaded with Co,N─C@MoS2 is introduced for the assembly of QDSCs. The incorporation of nanosized MoS2 enhances the density of catalytic sites, while the Co,N─C component ensures high conductivity and provides a substantial active surface area. Additionally, the titanium mesh's 3D structure serves as an effective electrical conduit, facilitating rapid electron transfer from the external circuit to the composite. These improvements in catalytic activity, charge transfer rate, and stability of the CE significantly enhance the photovoltaic performance of QDSCs. The optimized cells achieve a groundbreaking power conversion efficiency (PCE) of 16.39%, accompanied by a short-circuit current density (Jsc) of 27.26 mA cm-2, Voc of 0.818 V, and FF of 0.735. These results not only offer a new strategy for designing electrodes with high catalytic activity but also underscore the promising application of the Co,N─C@MoS2 composite in enhancing QDSC technology.

Intralayer/Interlayer Codoping Stabilizes Polarity Modulation in 2D Semiconductors for Scalable Electronics.

2D semiconductors show promise as a competitive candidate for developing future integrated circuits due to their immunity to short-channel effects and high carrier mobility at atomic layer thicknesses. The inherent defects and Fermi level pinning effect lead to n-type transport characteristics in most 2D semiconductors, while unstable and unsustainable p-type doping by various strategies hinders their application in many areas, such as complementary metal-oxide-semiconductor (CMOS) devices. In this study, an intralayer/interlayer codoping strategy is introduced that stabilizes p-type doping in 2D semiconductors. By incorporating oppositely charged ions (F and Li) with the intralayer/interlayer of 2D semiconductors, remarkable p-type doping in WSe2 and MoTe2 with air stability up to 9 months is achieved. Notably, the hole mobility presents a 100-fold enhancement (0.7 to 92 cm2 V-1 s-1) with the codoping procedure. Structural and elemental characterizations, combined with theoretical calculations validate the codoping mechanism. Moreover, a CMOS inverter and more complex logic functions such as NOR and XNOR, as well as large-area device arrays are demonstrated to showcase its applications and scalability. These findings suggest that stable and straightforward intralayer/interlayer codoping strategy with charge-space synergy holds the key to unlocking the potential of 2D semiconductors in complex and scalable device applications.

Epitaxy of wafer-scale single-crystal MoS2 monolayer via buffer layer control.

Monolayer molybdenum disulfide (MoS2), an emergent two-dimensional (2D) semiconductor, holds great promise for transcending the fundamental limits of silicon electronics and continue the downscaling of field-effect transistors. To realize its full potential and high-end applications, controlled synthesis of wafer-scale monolayer MoS2 single crystals on general commercial substrates is highly desired yet challenging. Here, we demonstrate the successful epitaxial growth of 2-inch single-crystal MoS2 monolayers on industry-compatible substrates of c-plane sapphire by engineering the formation of a specific interfacial reconstructed layer through the S/MoO3 precursor ratio control. The unidirectional alignment and seamless stitching of MoS2 domains across the entire wafer are demonstrated through cross-dimensional characterizations ranging from atomic- to centimeter-scale. The epitaxial monolayer MoS2 single crystal shows good wafer-scale uniformity and state-of-the-art quality, as evidenced from the ~100% phonon circular dichroism, exciton valley polarization of ~70%, room-temperature mobility of ~140 cm2v-1s-1, and on/off ratio of ~109. Our work provides a simple strategy to produce wafer-scale single-crystal 2D semiconductors on commercial insulator substrates, paving the way towards the further extension of Moore's law and industrial applications of 2D electronic circuits.

Phonon-enhanced nonlinearities in hexagonal boron nitride.

Polar crystals can be driven into collective oscillations by optical fields tuned to precise resonance frequencies. As the amplitude of the excited phonon modes increases, novel processes scaling non-linearly with the applied fields begin to contribute to the dynamics of the atomic system. Here we show two such optical nonlinearities that are induced and enhanced by the strong phonon resonance in the van der Waals crystal hexagonal boron nitride (hBN). We predict and observe large sub-picosecond duration signals due to four-wave mixing (FWM) during resonant excitation. The resulting FWM signal allows for time-resolved observation of the crystal motion. In addition, we observe enhancements of third-harmonic generation with resonant pumping at the hBN transverse optical phonon. Phonon-induced nonlinear enhancements are also predicted to yield large increases in high-harmonic efficiencies beyond the third.

Ultra-strong spin-orbit coupling and topological moiré engineering in twisted ZrS2 bilayers.

We predict that twisted bilayers of 1T-ZrS2 realize a novel and tunable platform to engineer two-dimensional topological quantum phases dominated by strong spin-orbit interactions. At small twist angles, ZrS2 heterostructures give rise to an emergent and twist-controlled moiré Kagome lattice, combining geometric frustration and strong spin-orbit coupling to give rise to a moiré quantum spin Hall insulator with highly controllable and nearly-dispersionless bands. We devise a generic pseudo-spin theory for group-IV transition metal dichalcogenides that relies on the two-component character of the valence band maximum of the 1T structure at Γ, and study the emergence of a robust quantum anomalous Hall phase as well as possible fractional Chern insulating states from strong Coulomb repulsion at fractional fillings of the topological moiré Kagome bands. Our results establish group-IV transition metal dichalcogenide bilayers as a novel moiré platform to realize strongly-correlated topological phases in a twist-tunable setting.