Intralayer charge-transfer moiré excitons in van der Waals superlattices.

Moiré patterns of transition metal dichalcogenide heterobilayers have proved to be an ideal platform on which to host unusual correlated electronic phases, emerging magnetism and correlated exciton physics. Whereas the existence of new moiré excitonic states is established1-4 through optical measurements, the microscopic nature of these states is still poorly understood, often relying on empirically fit models. Here, combining large-scale first-principles GW (where G and W denote the one-particle Green's function and the screened Coulomb interaction, respectively) plus Bethe-Salpeter calculations and micro-reflection spectroscopy, we identify the nature of the exciton resonances in WSe2/WS2 moiré superlattices, discovering a rich set of moiré excitons that cannot be captured by prevailing continuum models. Our calculations show moiré excitons with distinct characters, including modulated Wannier excitons and previously unidentified intralayer charge-transfer excitons. Signatures of these distinct excitonic characters are confirmed experimentally by the unique carrier-density and magnetic-field dependences of different moiré exciton resonances. Our study highlights the highly non-trivial exciton states that can emerge in transition metal dichalcogenide moiré superlattices, and suggests new ways of tuning many-body physics in moiré systems by engineering excited-states with specific spatial characters.

Efficient Fizeau drag from Dirac electrons in monolayer graphene.

Fizeau demonstrated in 1850 that the speed of light can be modified when it is propagating in moving media1. However, such control of the light speed has not been achieved efficiently with a fast-moving electron media by passing an electrical current. Because the strong electromagnetic coupling between the electron and light leads to the collective excitation of plasmon polaritons, it is hypothesized that Fizeau drag in electron flow systems manifests as a plasmonic Doppler effect. Experimental observation of the plasmonic Doppler effect in electronic systems has been challenge because the plasmon propagation speed is much faster than the electron drift velocity in conventional noble metals. Here we report direct observation of Fizeau drag of plasmon polaritons in strongly biased monolayer graphene by exploiting the high electron mobility and the slow plasmon propagation of massless Dirac electrons. The large bias current in graphene creates a fast-drifting Dirac electron medium hosting the plasmon polariton. This results in non-reciprocal plasmon propagation, where plasmons moving with the drifting electron media propagate at an enhanced speed. We measure the Doppler-shifted plasmon wavelength using cryogenic near-field infrared nanoscopy, which directly images the plasmon polariton mode in the biased graphene at low temperature. We observe a plasmon wavelength difference of up to 3.6 per cent between a plasmon moving with and a plasmon moving against the drifting electron media. Our findings on the plasmonic Doppler effect provide opportunities for electrical control of non-reciprocal surface plasmon polaritons in non-equilibrium systems.

Mott and generalized Wigner crystal states in WSe2/WS2 moiré superlattices.

Moiré superlattices can be used to engineer strongly correlated electronic states in two-dimensional van der Waals heterostructures, as recently demonstrated in the correlated insulating and superconducting states observed in magic-angle twisted-bilayer graphene and ABC trilayer graphene/boron nitride moiré superlattices1-4. Transition metal dichalcogenide moiré heterostructures provide another model system for the study of correlated quantum phenomena5 because of their strong light-matter interactions and large spin-orbit coupling. However, experimental observation of correlated insulating states in this system is challenging with traditional transport techniques. Here we report the optical detection of strongly correlated phases in semiconducting WSe2/WS2 moiré superlattices. We use a sensitive optical detection technique and reveal a Mott insulator state at one hole per superlattice site and surprising insulating phases at 1/3 and 2/3 filling of the superlattice, which we assign to generalized Wigner crystallization on the underlying lattice6-11. Furthermore, the spin-valley optical selection rules12-14 of transition metal dichalcogenide heterostructures allow us to optically create and investigate low-energy excited spin states in the Mott insulator. We measure a very long spin relaxation lifetime of many microseconds in the Mott insulating state, orders of magnitude longer than that of charge excitations. Our studies highlight the value of using moiré superlattices beyond graphene to explore correlated physics.

Author Correction: Observation of moiré excitons in WSe2/WS2 heterostructure superlattices.

Change history: In this Letter, the following text has been added to the Acknowledgements section: "the scanning transmission electron microscopy measurements at the Molecular Foundry were supported by the Office of Science, Office of Basic Energy Sciences, of the US Department of Energy under contract number DE-AC02-05CH11231". See accompanying Amendment.

Observation of moiré excitons in WSe2/WS2 heterostructure superlattices.

Moiré superlattices enable the generation of new quantum phenomena in two-dimensional heterostructures, in which the interactions between the atomically thin layers qualitatively change the electronic band structure of the superlattice. For example, mini-Dirac points, tunable Mott insulator states and the Hofstadter butterfly pattern can emerge in different types of graphene/boron nitride moiré superlattices, whereas correlated insulating states and superconductivity have been reported in twisted bilayer graphene moiré superlattices1-12. In addition to their pronounced effects on single-particle states, moiré superlattices have recently been predicted to host excited states such as moiré exciton bands13-15. Here we report the observation of moiré superlattice exciton states in tungsten diselenide/tungsten disulfide (WSe2/WS2) heterostructures in which the layers are closely aligned. These moiré exciton states manifest as multiple emergent peaks around the original WSe2 A exciton resonance in the absorption spectra, and they exhibit gate dependences that are distinct from that of the A exciton in WSe2 monolayers and in WSe2/WS2 heterostructures with large twist angles. These phenomena can be described by a theoretical model in which the periodic moiré potential is much stronger than the exciton kinetic energy and generates multiple flat exciton minibands. The moiré exciton bands provide an attractive platform from which to explore and control excited states of matter, such as topological excitons and a correlated exciton Hubbard model, in transition-metal dichalcogenides.

{SeO2(OH)} Bridging Lanthanide-Containing Antimono-Seleno-Tungstates.

A series of new trigonal pyramidal {SeO2(OH)} bridging lanthanide-containing antimono-seleno-tungstates [H2N(CH3)2]8Na8Cs4H9[Ln2SeW4O11(OH)(H2O)4(SbW9O33)(SeW9O33)(Se1/2Sb1/2W9O33)]2·32H2O [Ln = Tb (1), Dy (2), Ho (3), Er (4)] have been prepared by the synthetic strategy of simultaneously using the antimonotungstate precursor and simple material in an acidic aqueous solution and structurally characterized by single-crystal X-ray diffraction, powder X-ray diffraction, IR spectrometry, and thermogravimetric analysis. Their molecular structures contain an unprecedented hexameric polyoxoanion [Ln2SeW4O11(OH)(H2O)4(SbW9O33)(SeW9O33)(Se1/2Sb1/2W9O33)]229- constituted by two equivalent trimeric subunits Ln2W4O9(H2O)4(SbW9O33)(SeW9O33)(Se1/2Sb1/2W9O33) bridged via two µ2-{SeO2(OH)} linkers. Furthermore, the catalytic oxidation of various aromatic sulfides and sulfur mustard simulant 2-chloroethyl ethyl sulfide (CEES) by compound 3 as the heterogeneous catalyst has been investigated, exhibiting high conversion and selectivity as well as good stability and recyclability.

Floating-gate memristor based on a MoS2/h-BN/AuNPs mixed-dimensional heterostructure.

Memristors have recently received substantial attention because of its promising and unique application scenes emerging in neuromorphic computing which can achieve gains in computation speed by mimicking the topology of brains in electronic circuits. Traditional memristors made of bulk MoO3 and HfO2, etc. suffer from low switching ratio, short durability and poor stability. In this work, a floating-gate memristor is developed based on a mixed-dimensional heterostructure which is comprised of two-dimensional (2D) molybdenum disulfide (MoS2) and 0-dimensional (0D) Au nanoparticles (AuNPs) separated by an insulating hexagonal boron nitride (h-BN) layer, hereafter, MoS2/h-BN/AuNPs. We find that under the modulation of back-gate voltages, the MoS2/h-BN/AuNPs device operates reliably between a high resistance state (HRS) and a low resistance state (LRS) and that it shows multiple stable LRS states, demonstrating high potential of our memristor in application of multibit storage. The modulation effect can be attributed to the electron quantum tunneling between the AuNPs charge-trapping layer and MoS2 channel. Our memristor exhibits excellent durability and stability: the HRS and LRS remain more than 104 s without obvious degradation and the on/off ratio retains > 104 after more than 3000 switching cycles. We also demonstrate frequency-dependent memory properties upon electrical and optical pulse stimuli.

Layer-Dependent Interaction Effects in the Electronic Structure of Twisted Bilayer Graphene Devices.

Near the magic angle, strong correlations drive many intriguing phases in twisted bilayer graphene (tBG) including unconventional superconductivity and chern insulation. Whether correlations can tune symmetry breaking phases in tBG at intermediate (≳ 2°) twist angles remains an open fundamental question. Here, using ARPES, we study the effects of many-body interactions and displacement field on the band structure of tBG devices at an intermediate (3°) twist angle. We observe a layer- and doping-dependent renormalization of bands at the K points that is qualitatively consistent with moiré models of the Hartree-Fock interaction. We provide evidence of correlation-enhanced inversion symmetry-breaking, manifested by gaps at the Dirac points that are tunable with doping. These results suggest that electronic interactions play a significant role in the physics of tBG even at intermediate twist angles and present a new pathway toward engineering band structure and symmetry-breaking phases in moiré heterostructures.

2D Layered Materials for Fast-Charging Lithium-Ion Battery Anodes.

The development of electric vehicles has received worldwide attention in the background of reducing carbon emissions, wherein lithium-ion batteries (LIBs) become the primary energy supply systems. However, commercial graphite-based anodes in LIBs currently confront significant difficulty in enduring ultrahigh power input due to the slow Li+ transport rate and the low intercalation potential. This will, in turn, cause dramatic capacity decay and lithium plating. The 2D layered materials (2DLMs) recently emerge as new fast-charging anodes and hold huge promise for resolving the problems owing to the synergistic effect of a lower Li+ diffusion barrier, a proper Li+ intercalation potential, and a higher theoretical specific capacity with using them. In this review, the background and fundamentals of fast-charging for LIBs are first introduced. Then the research progress recently made for 2DLMs used for fast-charging anodes are elaborated and discussed. Some emerging research directions in this field with a short outlook on future studies are further discussed.

The dysfunction of hormone-sensitive lipase induces lipid deposition and reprogramming of nutrient metabolism in fish.

Hormone-sensitive lipase (HSL) is one of the rate-determining enzymes in the hydrolysis of TAG, playing a crucial role in lipid metabolism. However, the role of HSL-mediated lipolysis in systemic nutrient homoeostasis has not been intensively understood. Therefore, we used CRISPR/Cas9 technique and Hsl inhibitor (HSL-IN-1) to establish hsla-deficient (hsla-/-) and Hsl-inhibited zebrafish models, respectively. As a result, the hsla-/- zebrafish showed retarded growth and reduced oxygen consumption rate, accompanied with higher mRNA expression of the genes related to inflammation and apoptosis in liver and muscle. Furthermore, hsla-/- and HSL-IN-1-treated zebrafish both exhibited severe fat deposition, whereas their expressions of the genes related to lipolysis and fatty acid oxidation were markedly reduced. The TLC results also showed that the dysfunction of Hsl changed the whole-body lipid profile, including increasing the content of TG and decreasing the proportion of phospholipids. In addition, the systemic metabolic pattern was remodelled in hsla-/- and HSL-IN-1-treated zebrafish. The dysfunction of Hsl lowered the glycogen content in liver and muscle and enhanced the utilisation of glucose plus the expressions of glucose transporter and glycolysis genes. Besides, the whole-body protein content had significantly decreased in the hsla-/- and HSL-IN-1-treated zebrafish, accompanied with the lower activation of the mTOR pathway and enhanced protein and amino acid catabolism. Taken together, Hsl plays an essential role in energy homoeostasis, and its dysfunction would cause the disturbance of lipid catabolism but enhanced breakdown of glycogen and protein for energy compensation.

Excessive Iodine Enabled Ultrathin Inorganic Perovskite Growth at the Liquid-Air Interface.

The liquid-air interface offers a platform for the in-plane growth of free-standing materials. However, it is rarely used for inorganic perovskites and ultrathin non-layered perovskites. Herein the liquid-air interfacial synthesis of inorganic perovskite nanosheets (Cs3 Bi2 I9 , Cs3 Sb2 I9 ) is achieved simply by drop-casting the precursor solution with only the addition of iodine. The products are inaccessible without iodine addition. The thickness and lateral size of these nanosheets can be adjusted through the iodine concentration. The high volatility of the iodine spontaneously drives precursors that normally stay in the liquid to the liquid-air interface. The iodine also repairs in situ iodine vacancies during perovskite growth, giving enhanced optical and optoelectronic properties. The liquid-air interfacial growth of ultrathin perovskites provides multi-degree-of-freedom for constructing perovskite-based heterostructures and devices at atomic scale.

Engineering Fe and V Coordinated Bimetallic Oxide Nanocatalyst Enables Enhanced Polysulfides Mediation for High Energy Density Li-S Battery.

Lithium sulfur (Li-S) batteries are expected to become the next-generation rechargeable energy storage devices owing to their high theoretical energy density, environmental benignity, and economic benefits. However, the undesirable lithium polysulfides (LiPSs) shuttling and sluggish redox kinetics of sulfur electrochemistry severely degenerate the wide-ranging electrochemical performances, hindering the commercialization process of Li-S batteries. Herein, a Fe and V coordinated bimetallic oxide FeVO4 (denote FVO) nanocatalyst with three-dimensional (3D) ordered structure is thoughtfully tailored and cooperated with the commercialized carbon nanotubes (CNT) to modify polypropylene (PP) separator for achieving high efficiencies of restraining the LiPSs shuttling and boosting the redox conversion of sulfur species. The Fe and V coordinated bimetallic oxide demonstrates enhanced anchoring and catalyzing activities toward sulfur species than single metal oxides of Fe and V with homometallic valence states due to the reconfiguration of the 3d-band. Impressively, the Li-S pouch cell with the FVO/CNT@PP separator achieves an energy density up to 341 Wh kg-1 . The bimetallic oxide nanocatalyst used in this work enlightens a new designing route toward the separator modification for the development of high energy density Li-S batteries.

Imaging moiré flat bands in three-dimensional reconstructed WSe2/WS2 superlattices.

Moiré superlattices in transition metal dichalcogenide (TMD) heterostructures can host novel correlated quantum phenomena due to the interplay of narrow moiré flat bands and strong, long-range Coulomb interactions1-9. However, microscopic knowledge of the atomically reconstructed moiré superlattice and resulting flat bands is still lacking, which is critical for fundamental understanding and control of the correlated moiré phenomena. Here we quantitatively study the moiré flat bands in three-dimensional (3D) reconstructed WSe2/WS2 moiré superlattices by comparing scanning tunnelling spectroscopy (STS) of high-quality exfoliated TMD heterostructure devices with ab initio simulations of TMD moiré superlattices. A strong 3D buckling reconstruction accompanied by large in-plane strain redistribution is identified in our WSe2/WS2 moiré heterostructures. STS imaging demonstrates that this results in a remarkably narrow and highly localized K-point moiré flat band at the valence band edge of the heterostructure. A series of moiré flat bands are observed at different energies that exhibit varying degrees of localization. Our observations contradict previous simplified theoretical models but agree quantitatively with ab initio simulations that fully capture the 3D structural reconstruction. Our results reveal that the strain redistribution and 3D buckling in TMD heterostructures dominate the effective moiré potential and the corresponding moiré flat bands at the Brillouin zone K points.

A Multi-Scale Study on Deformation and Failure Process of Metallic Structures in Extreme Environment.

It is a macro-micro model study for defect initiation, growth and crack propagation of metallic truss structure under high engine temperature and pressure conditions during the reentry atmosphere. Till now, the multi-scale simulation methods for these processes are still unclear. We explore the deformation and failure processes from macroscale to nanoscale using the Gas-Kinetic Unified Algorithm (GKUA) and all-atomic, molecular dynamic (MD) simulation method. The behaviors of the dislocations, defect evolution and crack propagation until failure for Aluminum-Magnesium (Al-Mg) alloy are considered with the different temperature background and strain fields. The results of distributions of temperature and strain field in the aerodynamic environment obtained by molecular dynamics simulations are in good agreement with those obtained from the macroscopic Boltzmann method. Compared to the tensile loading, the alloy structure is more sensitive to compression loading. The polycrystalline Al-Mg alloy has higher yield strength with a larger grain size. It is due to the translation of plastic deformation mode from grain boundary (GB) sliding to dislocation slip and the accumulation of dislocation line. Our findings have paved a new way to analyze and predict the metallic structural failure by micro-scale analysis under the aerodynamic thermal extreme environment of the reentry spacecraft on service expiration.

Nonlinear Luttinger liquid plasmons in semiconducting single-walled carbon nanotubes.

Interacting electrons confined in one dimension are generally described by the Luttinger liquid formalism, where the low-energy electronic dispersion is assumed to be linear and the resulting plasmonic excitations are non-interacting. Instead, a Luttinger liquid in one-dimensional materials with nonlinear electronic bands is expected to show strong plasmon-plasmon interactions, but an experimental demonstration of this behaviour has been lacking. Here, we combine infrared nano-imaging and electronic transport to investigate the behaviour of plasmonic excitations in semiconducting single-walled carbon nanotubes with carrier density controlled by electrostatic gating. We show that both the propagation velocity and the dynamic damping of plasmons can be tuned continuously, which is well captured by the nonlinear Luttinger liquid theory. These results contrast with the gate-independent plasmons observed in metallic nanotubes, as expected for a linear Luttinger liquid. Our findings provide an experimental demonstration of one-dimensional electron dynamics beyond the conventional linear Luttinger liquid paradigm and are important for understanding excited-state properties in one dimension.

Infrared Light-Emitting Devices from Antenna-Coupled Luttinger Liquid Plasmons In Carbon Nanotubes.

Electrically driven light-emitting devices provide highly energy-efficient lighting at visible wavelengths, and they have transformed photonic and electronic lighting applications. Efficient infrared light-emitting devices, however, have been challenging because band gap emission from semiconductors becomes inefficient in the mid-infrared to far-infrared spectral range. Here we investigate infrared light-emitting devices (IRLEDs) based on Luttinger liquid (LL) plasmons in one-dimensional (1D) metallic carbon nanotubes. Elementary excitations in LL are characterized by collective charge and spin excitations, i.e., plasmons and spinons. Consequently, electrons injected into the nanotubes transform efficiently into LL plasmons, a hybrid excitation of electromagnetic fields and electrons. We design nanoantennas coupled to the carbon nanotube to radiate LL plasmons into the far field. LL-based IRLEDs can be designed to selectively emit at wavelengths across the far- and mid-infrared spectra. An electrical-to-optical power conversion efficiency up to 3.2% may be achieved. Such efficient and narrowband LL-based IRLEDs can enable novel infrared nanophotonic applications.

Soliton-Dependent Electronic Transport across Bilayer Graphene Domain Wall.

Layer-stacking domain wall in bilayer graphene is one type of topological defects that can greatly affect the electronic properties of bilayer graphene and therefore lead to nontrivial transport behaviors. An outstanding question on the layer stacking domain wall is how the electrons hop between two adjacent stacking domains. Here we report the first experimental observation of electronic transport across bilayer graphene domain walls by combining near-field infrared nanoscopy and scanning voltage microscopy techniques. We observe markedly different electron transport behaviors across the tensile- and shear-type domain walls. The tensile-type domain wall is highly reflective of low-energy incident electrons, but becomes more transparent when the electron density and the Fermi energy are increased by electrostatic gating. In contrast, the shear-type domain wall is always highly transparent at different gate voltages. Such soliton-dependent electronic transport can open up new routes to engineer novel nanoelectronic devices based on layer-stacking domain walls in bilayer graphene.

Global Control of Stacking-Order Phase Transition by Doping and Electric Field in Few-Layer Graphene.

The layer stacking order has profound effects on the physical properties of two-dimensional van der Waals heterostructures. For example, graphene multilayers can have distinct electronic band structures and exhibit completely different behaviors depending on the stacking order. Fascinating physical phenomena, such as correlated insulators, superconductors, and ferromagnetism, can also emerge with a periodic variation of the layer stacking order, which is known as the moiré superlattice in van der Waals materials. In this work, we realize the global phase transition between different graphene layer stacking orders and elucidate its microscopic origin. We experimentally determine the energy difference between different stacking orders with the accuracy of µeV/atom. We reveal that both the carrier doping and the electric field can drive the layer-stacking phase transition through different mechanisms: carrier doping can change the energy difference because of a non-negligible work function difference between different stacking orders; the electric field, on the other hand, induces a band-gap opening in ABC-stacked graphene and hence changes the energy difference. Our findings provide a fundamental understanding of the electrically driven stacking-order phase transition in few-layer graphene and demonstrate a reversible and noninvasive method to globally control the stacking order.

Tunneling Spectroscopy in Carbon Nanotube-Hexagonal Boron Nitride-Carbon Nanotube Heterojunctions.

Electron tunneling spectroscopy is a powerful technique to probe the unique physical properties of one-dimensional (1D) single-walled carbon nanotubes (SWNTs), such as the van Hove singularities in the density of states or the power-law tunneling probability of a Luttinger liquid. However, little is known about the tunneling behavior between two 1D SWNTs over a large energy spectrum. Here, we investigate the electron tunneling behavior between two crossed SWNTs across a wide spectral window up to 2 eV in the unique carbon nanotube-hexagonal boron nitride-carbon nanotube heterojunctions. We observe many sharp resonances in the differential tunneling conductance at different bias voltages applied between the SWNTs. These resonances can be attributed to elastic tunneling into the van Hove singularities of different 1D subbands in both SWNTs, and they allow us to determine the quasi-particle bandgaps and higher-lying 1D subbands in SWNTs on the insulating substrate.

Optical Imaging and Spectroscopy of Atomically Precise Armchair Graphene Nanoribbons.

We report the optical imaging and absorption spectroscopy on atomically precise armchair graphene nanoribbons (GNRs) on insulating fused silica substrates. This is achieved by controlling light polarization on macroscopically aligned GNRs which greatly enhances the optical contrast of the submonolayer GNRs on the insulating substrates. We measure the linear absorption spectra of 7-armchair and 9-armchair GNRs in this study, and the experimental data agree qualitatively with ab inito calculation results. The polarization spectroscopy technique enables an unambiguous optical identification of GNRs and provides a rapid tool to characterize the transferred film over a large area.