Tunable electron-flexural phonon interaction in graphene heterostructures.

Peculiar electron-phonon interaction characteristics underpin the ultrahigh mobility1, electron hydrodynamics2-4, superconductivity5 and superfluidity6,7 observed in graphene heterostructures. The Lorenz ratio between the electronic thermal conductivity and the product of the electrical conductivity and temperature provides insight into electron-phonon interactions that is inaccessible to past graphene measurements. Here we show an unusual Lorenz ratio peak in degenerate graphene near 60 kelvin and decreased peak magnitude with increased mobility. When combined with ab initio calculations of the many-body electron-phonon self-energy and analytical models, this experimental observation reveals that broken reflection symmetry in graphene heterostructures can relax a restrictive selection rule8,9 to allow quasielastic electron coupling with an odd number of flexural phonons, contributing to the increase of the Lorenz ratio towards the Sommerfeld limit at an intermediate temperature sandwiched between the low-temperature hydrodynamic regime and the inelastic electron-phonon scattering regime above 120 kelvin. In contrast to past practices of neglecting the contributions of flexural phonons to transport in two-dimensional materials, this work suggests that tunable electron-flexural phonon couping can provide a handle to control quantum matter at the atomic scale, such as in magic-angle twisted bilayer graphene10 where low-energy excitations may mediate Cooper pairing of flat-band electrons11,12.

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.

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.

Magnetic and magnetic inverse spin Hall effects in a non-collinear antiferromagnet.

The spin Hall effect (SHE)1-5 achieves coupling between charge currents and collective spin dynamics in magnetically ordered systems and is a key element of modern spintronics6-9. However, previous research has focused mainly on non-magnetic materials, so the magnetic contribution to the SHE is not well understood. Here we show that antiferromagnets have richer spin Hall properties than do non-magnetic materials. We find that in the non-collinear antiferromagnet10 Mn3Sn, the SHE has an anomalous sign change when its triangularly ordered moments switch orientation. We observe contributions to the SHE (which we call the magnetic SHE) and the inverse SHE (the magnetic inverse SHE) that are absent in non-magnetic materials and that can be dominant in some magnetic materials, including antiferromagnets. We attribute the dominance of this magnetic mechanism in Mn3Sn to the momentum-dependent spin splitting that is produced by non-collinear magnetic order. This discovery expands the horizons of antiferromagnet spintronics and spin-charge coupling mechanisms.

Publisher Correction: Magnetic and magnetic inverse spin Hall effects in a non-collinear antiferromagnet.

In this Letter, the formatting of some of the crystallographic axes was incorrect. This has been corrected online.

Superconductors, orbital magnets and correlated states in magic-angle bilayer graphene.

Superconductivity can occur under conditions approaching broken-symmetry parent states1. In bilayer graphene, the twisting of one layer with respect to the other at 'magic' twist angles of around 1 degree leads to the emergence of ultra-flat moiré superlattice minibands. Such bands are a rich and highly tunable source of strong-correlation physics2-5, notably superconductivity, which emerges close to interaction-induced insulating states6,7. Here we report the fabrication of magic-angle twisted bilayer graphene devices with highly uniform twist angles. The reduction in twist-angle disorder reveals the presence of insulating states at all integer occupancies of the fourfold spin-valley degenerate flat conduction and valence bands-that is, at moiré band filling factors ν = 0, ±1, ±2, ±3. At ν ≈ -2, superconductivity is observed below critical temperatures of up to 3 kelvin. We also observe three new superconducting domes at much lower temperatures, close to the ν = 0 and ν = ±1 insulating states. Notably, at ν = ± 1 we find states with non-zero Chern numbers. For ν = -1 the insulating state exhibits a sharp hysteretic resistance enhancement when a perpendicular magnetic field greater than 3.6 tesla is applied, which is consistent with a field-driven phase transition. Our study shows that broken-symmetry states, interaction-driven insulators, orbital magnets, states with non-zero Chern numbers and superconducting domes occur frequently across a wide range of moiré flat band fillings, including close to charge neutrality. This study provides a more detailed view of the phenomenology of magic-angle twisted bilayer graphene, adding to our evolving understanding of its emergent properties.

Evidence for moiré excitons in van der Waals heterostructures.

Recent advances in the isolation and stacking of monolayers of van der Waals materials have provided approaches for the preparation of quantum materials in the ultimate two-dimensional limit1,2. In van der Waals heterostructures formed by stacking two monolayer semiconductors, lattice mismatch or rotational misalignment introduces an in-plane moiré superlattice3. It is widely recognized that the moiré superlattice can modulate the electronic band structure of the material and lead to transport properties such as unconventional superconductivity4 and insulating behaviour driven by correlations5-7; however, the influence of the moiré superlattice on optical properties has not been investigated experimentally. Here we report the observation of multiple interlayer exciton resonances with either positive or negative circularly polarized emission in a molybdenum diselenide/tungsten diselenide (MoSe2/WSe2) heterobilayer with a small twist angle. We attribute these resonances to excitonic ground and excited states confined within the moiré potential. This interpretation is supported by recombination dynamics and by the dependence of these interlayer exciton resonances on twist angle and temperature. These results suggest the feasibility of engineering artificial excitonic crystals using van der Waals heterostructures for nanophotonics and quantum information applications.

Visualizing the interplay of Dirac mass gap and magnetism at nanoscale in intrinsic magnetic topological insulators.

In intrinsic magnetic topological insulators, Dirac surface-state gaps are prerequisites for quantum anomalous Hall and axion insulating states. Unambiguous experimental identification of these gaps has proved to be a challenge, however. Here, we use molecular beam epitaxy to grow intrinsic MnBi2Te4 thin films. Using scanning tunneling microscopy/spectroscopy, we directly visualize the Dirac mass gap and its disappearance below and above the magnetic order temperature. We further reveal the interplay of Dirac mass gaps and local magnetic defects. We find that, in high defect regions, the Dirac mass gap collapses. Ab initio and coupled Dirac cone model calculations provide insight into the microscopic origin of the correlation between defect density and spatial gap variations. This work provides unambiguous identification of the Dirac mass gap in MnBi2Te4 and, by revealing the microscopic origin of its gap variation, establishes a material design principle for realizing exotic states in intrinsic magnetic topological insulators.

Layer-dependent correlated phases in WSe2/MoS2 moiré superlattice.

Electron correlation plays an essential role in the macroscopic quantum phenomena in the moiré heterostructure, such as antiferromagnetism and correlated insulating phases. Unlike the phenomena where the interaction involves only electrons in one layer, the interaction of distinct phases in two or more layers represents a new horizon forward, such as the one in the Kondo lattice model. Here, using interlayer excitons as a probe, we show that the interlayer interactions in heterobilayers of tungsten diselenide and molybdenum disulfide (WSe2/MoS2) can be electrically switched on and off, resulting in a layer-dependent correlated phase diagram, including single-layer, layer-selective, excitonic-insulator and layer-hybridized regions. We demonstrate that these correlated phases affect the interlayer exciton non-radiative decay pathways. These results reveal the role of strong correlation on interlayer exciton dynamics and pave the way for studying the layer-resolved strong correlation behaviour in moiré heterostructures.

Magic Angles and Fractional Chern Insulators in Twisted Homobilayer Transition Metal Dichalcogenides.

We explain the appearance of magic angles and fractional Chern insulators in twisted K-valley homobilayer transition metal dichalcogenides by mapping their continuum model to a Landau level problem. Our approach relies on an adiabatic approximation for the quantum mechanics of valence band holes in a layer-pseudospin field that is valid for sufficiently small twist angles and on a lowest Landau level approximation that is valid for sufficiently large twist angles. It provides a simple qualitative explanation for the nearly ideal quantum geometry of the lowest moiré miniband at particular twist angles, predicts that topological flat bands occur only when the valley-dependent moiré potential is sufficiently strong compared to the interlayer tunneling amplitude, and provides a convenient starting point for the study of interactions.

Exchange-Driven Chern States in High-Mobility Intrinsic Magnetic Topological Insulators.

The layer-dependent Chern number (C) in MnBi_{2}Te_{4} is characterized by the presence of a Weyl semimetal state in the ferromagnetic coupling. However, the influence of a key factor, namely, the exchange coupling, remains unexplored. This study focuses on characterizing the C=2 state in MnBi_{2}Te_{4}, which is classified as a higher C state resulting from the anomalous n=0 Landau levels (LLs). Our findings demonstrate that the exchange coupling parameter strongly influences the formation of this Chern state, leading to a competition between the C=1 and 2 states. Moreover, the emergence of odd-even LL sequences, resulting from the breaking of LL degeneracy, provides compelling evidence for the strong exchange coupling strength. These findings highlight the significance of the exchange coupling in understanding the behavior of Chern states and LLs in magnetic quantum systems.

Γ valley transition metal dichalcogenide moiré bands.

The valence band maxima of most group VI transition metal dichalcogenide thin films remain at the Γ point all of the way from bulk to bilayer. In this paper, we develop a continuum theory of the moiré minibands that are formed in the valence bands of Γ-valley homobilayers by a small relative twist. Our effective theory is benchmarked against large-scale ab initio electronic structure calculations that account for lattice relaxation. As a consequence of an emergent [Formula: see text] symmetry, we find that low-energy Γ-valley moiré holes differ qualitatively from their K-valley counterparts addressed previously; in energetic order, the first three bands realize 1) a single-orbital model on a honeycomb lattice, 2) a two-orbital model on a honeycomb lattice, and 3) a single-orbital model on a kagome lattice.

Multiple flat bands and topological Hofstadter butterfly in twisted bilayer graphene close to the second magic angle.

Moiré superlattices in two-dimensional van der Waals heterostructures provide an efficient way to engineer electron band properties. The recent discovery of exotic quantum phases and their interplay in twisted bilayer graphene (tBLG) has made this moiré system one of the most renowned condensed matter platforms. So far studies of tBLG have been mostly focused on the lowest two flat moiré bands at the first magic angle θm1 ∼ 1.1°, leaving high-order moiré bands and magic angles largely unexplored. Here we report an observation of multiple well-isolated flat moiré bands in tBLG close to the second magic angle θm2 ∼ 0.5°, which cannot be explained without considering electron-election interactions. With high magnetic field magnetotransport measurements we further reveal an energetically unbound Hofstadter butterfly spectrum in which continuously extended quantized Landau level gaps cross all trivial band gaps. The connected Hofstadter butterfly strongly evidences the topologically nontrivial textures of the multiple moiré bands. Overall, our work provides a perspective for understanding the quantum phases in tBLG and the fractal Hofstadter spectra of multiple topological bands.

Functional Renormalization Group Study of Superconductivity in Rhombohedral Trilayer Graphene.

We employ a functional renormalization group approach to ascertain the pairing mechanism and symmetry of the superconducting phase observed in rhombohedral trilayer graphene. Superconductivity in this system occurs in a regime of carrier density and displacement field with a weakly distorted annular Fermi sea. We find that repulsive Coulomb interactions can induce electron pairing on the Fermi surface by taking advantage of momentum-space structure associated with the finite width of the Fermi sea annulus. The degeneracy between spin-singlet and spin-triplet pairing is lifted by valley-exchange interactions that strengthen under the RG flow and develop nontrivial momentum-space structure. We find that the leading pairing instability is d-wave-like and spin singlet, and that the theoretical phase diagram versus carrier density and displacement field agrees qualitatively with experiment.

Magnetized topological insulator multilayers.

We discuss the magnetic and topological properties of bulk crystals and quasi-two-dimensional (quasi-2D) thin films formed by stacking intrinsic magnetized topological insulator (for example, Mn ([Formula: see text])2X4 with X = Se,Te) septuple layers and topological insulator quintuple layers in arbitrary order. Our analysis makes use of a simplified model that retains only Dirac cone degrees of freedom on both surfaces of each septuple or quintuple layer. We demonstrate the model's applicability and estimate its parameters by comparing with ab initio density-functional theory (DFT) calculations. We then employ the coupled Dirac cone model to provide an explanation for the dependence of thin-film properties, particularly the presence or absence of the quantum anomalous Hall effect, on film thickness, magnetic configuration, and stacking arrangement, and to comment on the design of Weyl superlattices.

Unveiling defect-mediated carrier dynamics in monolayer semiconductors by spatiotemporal microwave imaging.

The optoelectronic properties of atomically thin transition-metal dichalcogenides are strongly correlated with the presence of defects in the materials, which are not necessarily detrimental for certain applications. For instance, defects can lead to an enhanced photoconduction, a complicated process involving charge generation and recombination in the time domain and carrier transport in the spatial domain. Here, we report the simultaneous spatial and temporal photoconductivity imaging in two types of WS2 monolayers by laser-illuminated microwave impedance microscopy. The diffusion length and carrier lifetime were directly extracted from the spatial profile and temporal relaxation of microwave signals, respectively. Time-resolved experiments indicate that the critical process for photoexcited carriers is the escape of holes from trap states, which prolongs the apparent lifetime of mobile electrons in the conduction band. As a result, counterintuitively, the long-lived photoconductivity signal is higher in chemical-vapor deposited (CVD) samples than exfoliated monolayers due to the presence of traps that inhibits recombination. Our work reveals the intrinsic time and length scales of electrical response to photoexcitation in van der Waals materials, which is essential for their applications in optoelectronic devices.

Confined Monolayer Ag As a Large Gap 2D Semiconductor and Its Momentum Resolved Excited States.

2D materials have intriguing quantum phenomena that are distinctively different from their bulk counterparts. Recently, epitaxially synthesized wafer-scale 2D metals, composed of elemental atoms, are attracting attention not only for their potential applications but also for exotic quantum effects such as superconductivity. By mapping momentum-resolved electronic states using time-resolved and angle-resolved photoemission spectroscopy (ARPES), we reveal that monolayer Ag confined between bilayer graphene and SiC is a large gap (>1 eV) 2D semiconductor, consistent with ab initio GW calculations. The measured valence band dispersion matches the GW quasiparticle band structure. However, the conduction band dispersion shows an anomalously large effective mass of 2.4 m0. Possible mechanisms for this large enhancement in the "apparent mass" are discussed.

Phonon renormalization in reconstructed MoS2 moiré superlattices.

In moiré crystals formed by stacking van der Waals materials, surprisingly diverse correlated electronic phases and optical properties can be realized by a subtle change in the twist angle. Here, we discover that phonon spectra are also renormalized in MoS2 twisted bilayers, adding an insight to moiré physics. Over a range of small twist angles, the phonon spectra evolve rapidly owing to ultra-strong coupling between different phonon modes and atomic reconstructions of the moiré pattern. We develop a low-energy continuum model for phonons that overcomes the outstanding challenge of calculating the properties of large moiré supercells and successfully captures the essential experimental observations. Remarkably, simple optical spectroscopy experiments can provide information on strain and lattice distortions in moiré crystals with nanometre-size supercells. The model promotes a comprehensive and unified understanding of the structural, optical and electronic properties of moiré superlattices.

Nonlocal Interactions in Moiré Hubbard Systems.

Moiré materials formed in two-dimensional semiconductor heterobilayers are quantum simulators of Hubbard-like physics with unprecedented electron density and interaction strength tunability. Compared to atomic scale Hubbard-like systems, electrons or holes in moiré materials are less strongly attracted to their effective lattice sites because these are defined by finite-depth potential extrema. As a consequence, nonlocal interaction terms like interaction-assisted hopping and intersite exchange are more relevant. We theoretically demonstrate the possibility of tuning the strength of these coupling constants to favor unusual states of matter, including spin liquids, insulating ferromagnets, and superconductors.

Pseudospin Paramagnons and the Superconducting Dome in Magic Angle Twisted Bilayer Graphene.

We present a theory of superconductivity in twisted bilayer graphene in which attraction is generated between electrons on the same honeycomb sublattice when the system is close to a sublattice polarization instability. The resulting Cooper pairs are spin-polarized valley singlets. Because the sublattice polarizability is mainly contributed by interband fluctuations, superconductivity occurs over a wide range of filling fraction. It is suppressed by (i) applying a sublattice polarizing field (generated by an aligned BN substrate) or (ii) changing moiré band filling to favor valley polarization. The enhanced intrasublattice attraction close to sublattice polarization instability is analogous to enhanced like-spin attraction in liquid ^{3}He near the melting curve and the enhanced valley-singlet repulsion close to valley-polarization instabilities is analogous to enhanced spin-singlet repulsion in metals that are close to a ferromagnetic instability. We comment on the relationship between our pseudospin paramagnon model and the rich phenomenology of superconductivity in twisted bilayer and multilayer graphene.