Tuning commensurability in twisted van der Waals bilayers.

Moiré superlattices based on van der Waals bilayers1-4 created at small twist angles lead to a long wavelength pattern with approximate translational symmetry. At large twist angles (θt), moiré patterns are, in general, incommensurate except for a few discrete angles. Here we show that large-angle twisted bilayers offer distinctly different platforms. More specifically, by using twisted tungsten diselenide bilayers, we create the incommensurate dodecagon quasicrystals at θt = 30° and the commensurate moiré crystals at θt = 21.8° and 38.2°. Valley-resolved scanning tunnelling spectroscopy shows disparate behaviours between moiré crystals (with translational symmetry) and quasicrystals (with broken translational symmetry). In particular, the K valley shows rich electronic structures exemplified by the formation of mini-gaps near the valence band maximum. These discoveries demonstrate that bilayers with large twist angles offer a design platform to explore moiré physics beyond those formed with small twist angles.

Electrostatic moiré potential from twisted hexagonal boron nitride layers.

Moiré superlattices host a rich variety of correlated electronic phases. However, the moiré potential is fixed by interlayer coupling, and it is dependent on the nature of carriers and valleys. In contrast, it has been predicted that twisted hexagonal boron nitride (hBN) layers can impose a periodic electrostatic potential capable of engineering the properties of adjacent functional layers. Here, we show that this potential is described by a theory of electric polarization originating from the interfacial charge redistribution, validated by its dependence on supercell sizes and distance from the twisted interfaces. This enables controllability of the potential depth and profile by controlling the twist angles between the two interfaces. Employing this approach, we further demonstrate how the electrostatic potential from a twisted hBN substrate impedes exciton diffusion in semiconductor monolayers, suggesting opportunities for engineering the properties of adjacent functional layers using the surface potential of a twisted hBN substrate.

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.

Remarkably Deep Moiré Potential for Intralayer Excitons in MoSe2/MoS2 Twisted Heterobilayers.

A moiré superlattice formed in twisted van der Waals bilayers has emerged as a new tuning knob for creating new electronic states in two-dimensional materials. Excitonic properties can also be altered drastically due to the presence of moiré potential. However, quantifying the moiré potential for excitons is nontrivial. By creating a large ensemble of MoSe2/MoS2 heterobilayers with a systematic variation of twist angles, we map out the minibands of interlayer and intralayer excitons as a function of twist angles, from which we determine the moiré potential for excitons. Surprisingly, the moiré potential depth for intralayer excitons is up to ∼130 meV, comparable to that for interlayer excitons. This result is markedly different from theoretical calculations based on density functional theory, which show an order of magnitude smaller moiré potential for intralayer excitons. The remarkably deep intralayer moiré potential is understood within the framework of structural reconstruction within the moiré unit cell.

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.

Time-resolved ARPES Determination of a Quasi-Particle Band Gap and Hot Electron Dynamics in Monolayer MoS2.

The electronic structure and dynamics of 2D transition metal dichalcogenide (TMD) monolayers provide important underpinnings both for understanding the many-body physics of electronic quasi-particles and for applications in advanced optoelectronic devices. However, extensive experimental investigations of semiconducting monolayer TMDs have yielded inconsistent results for a key parameter, the quasi-particle band gap (QBG), even for measurements carried out on the same layer and substrate combination. Here, we employ sensitive time- and angle-resolved photoelectron spectroscopy (trARPES) for a high-quality large-area MoS2 monolayer to capture its momentum-resolved equilibrium and excited-state electronic structure in the weak-excitation limit. For monolayer MoS2 on graphite, we obtain QBG values of ≈2.10 eV at 80 K and of ≈2.03 eV at 300 K, results well-corroborated by the scanning tunneling spectroscopy (STS) measurements on the same material.

Engineering Giant Rabi Splitting via Strong Coupling between Localized and Propagating Plasmon Modes on Metal Surface Lattices: Observation of √N Scaling Rule.

We present a strong coupling system realized by coupling the localized surface plasmon mode in individual silver nanogrooves and propagating surface plasmon modes launched by periodic nanogroove arrays with varied periodicities on a continuous silver medium. When the propagating modes are in resonance with the localized mode, we observe a √N scaling of Rabi splitting energy, where N is the number of propagating modes coupled to the localized mode. Here, we confirm a giant Rabi splitting on the order of 450-660 meV (N = 2) in the visible spectral range, and the corresponding coupling strength is 160-235 meV. In some of the strong coupling cases studied by us, the coupling strength is about 10% of the mode energy, reaching the ultrastrong coupling regime.

Tuning of Two-Dimensional Plasmon-Exciton Coupling in Full Parameter Space: A Polaritonic Non-Hermitian System.

Non-Hermitian photonic systems with gains and/or losses have recently emerged as a powerful approach for topology-protected optical transport and novel device applications. To date, most of these systems employ coupled optical systems of diffraction-limited dielectric waveguides or microcavities, which exchange energy spatially or temporally. Here, we introduce a diffraction-unlimited approach using a plasmon-exciton coupling (polariton) system with tunable plasmonic resonance (energy and line width) and coupling strength. By designing a chirped silver nanogroove cavity array and coupling a single tungsten disulfide monolayer with a large contrast in resonance line width, we show the tuning capability through energy level anticrossing and plasmon-exciton hybridization (line width crossover), as well as spontaneous symmetry breaking across the exceptional point at zero detuning. This two-dimensional hybrid material system can be applied as a scalable and integratable platform for non-Hermitian photonics, featuring seamless integration of two-dimensional materials, broadband tuning, and operation at room temperature.

Influence of Nanosize Hole Defects and their Geometric Arrangements on the Superfluid Density in Atomically Thin Single Crystals of Indium Superconductor.

Using Indium sqrt[7]×sqrt[3] on Si(111) as an atomically thin superconductor platform, and by systematically controlling the density of nanohole defects (nanometer size voids), we reveal the impacts of defect density and defect geometric arrangements on superconductivity at macroscopic and microscopic length scales. When nanohole defects are uniformly dispersed in the atomic layer, the superfluid density monotonically decreases as a function of defect density (from 0.7% to 5% of the surface area) with minor change in the transition temperature T_{C}, measured both microscopically and macroscopically. With a slight increase in the defect density from 5% to 6%, these point defects are organized into defect chains that enclose individual two-dimensional patches. This new geometric arrangement of defects dramatically impacts the superconductivity, leading to the total disappearance of macroscopic superfluid density and the collapse of the microscopic superconducting gap. This study sheds new light on the understanding of how local defects and their geometric arrangements impact superconductivity in the two-dimensional limit.

PTCDA Molecular Monolayer on Pb Thin Films: An Unusual π-Electron Kondo System and Its Interplay with a Quantum-Confined Superconductor.

The hybridization of magnetism and superconductivity has been an intriguing playground for correlated electron systems, hosting various novel physical phenomena. Usually, localized d or f electrons are central to magnetism. In this study, by placing a PTCDA (3,4,9,10-perylene tetracarboxylic dianhydride) molecular monolayer on ultrathin Pb films, we built a hybrid magnetism/superconductivity (M/SC) system consisting of only sp electronic levels. The magnetic moments reside in the unpaired molecular orbital originating from interfacial charge transfers. We reported distinctive tunneling spectroscopic features of such a Kondo screened π electron impurity lattice on a superconductor in the regime of T_{K}≫Δ, suggesting the formation of a two-dimensional bound states band. Moreover, moiré superlattices with tunable twist angle and the quantum confinement in the ultrathin Pb films provide easy and flexible implementations to tune the interplay between the Kondo physics and the superconductivity, which are rarely present in M/SC hybrid systems.

Ultrathin two-dimensional superconductivity with strong spin-orbit coupling.

We report on a study of epitaxially grown ultrathin Pb films that are only a few atoms thick and have parallel critical magnetic fields much higher than the expected limit set by the interaction of electron spins with a magnetic field, that is, the Clogston-Chandrasekhar limit. The epitaxial thin films are classified as dirty-limit superconductors because their mean-free paths, which are limited by surface scattering, are smaller than their superconducting coherence lengths. The uniformity of superconductivity in these thin films is established by comparing scanning tunneling spectroscopy, scanning superconducting quantum interference device (SQUID) magnetometry, double-coil mutual inductance, and magneto-transport, data that provide average superfluid rigidity on length scales covering the range from microscopic to macroscopic. We argue that the survival of superconductivity at Zeeman energies much larger than the superconducting gap can be understood only as the consequence of strong spin-orbit coupling that, together with substrate-induced inversion-symmetry breaking, produces spin splitting in the normal-state energy bands that is much larger than the superconductor's energy gap.

Giant Enhancement of Defect-Bound Exciton Luminescence and Suppression of Band-Edge Luminescence in Monolayer WSe2-Ag Plasmonic Hybrid Structures.

We have investigated how the photoluminescence (PL) of WSe2 is modified when coupled to Ag plasmonic structures at low temperature. Chemical vapor deposition (CVD) grown monolayer WSe2 flakes were transferred onto a Ag film and a Ag nanotriangle array that had a 1.5 nm Al2O3 capping layer. Using low-temperature (7.5 K) micro-PL mapping, we simultaneously observed enhancement of the defect-bound exciton emission and quenching of the band edge exciton emission when the WSe2 was on a plasmonic structure. The enhancement of the defect-bound exciton emission was significant with enhancement factors of up to ∼200 for WSe2 on the nanotriangle array when compared to WSe2 on a 1.5 nm Al2O3 capped Si substrate with a 300 nm SiO2 layer. The giant enhancement of the luminescence from the defect-bound excitons is understood in terms of the Purcell effect and increased light absorption. In contrast, the surprising result of luminescence quenching of the bright exciton state on the same plasmonic nanostructure is due to a rather unique electronic structure of WSe2: the existence of a dark state below the bright exciton state.

Contrasting Structural Reconstructions, Electronic Properties, and Magnetic Orderings along Different Edges of Zigzag Transition Metal Dichalcogenide Nanoribbons.

Two-dimensional transition metal dichalcogenides represent an emerging class of layered materials exhibiting various intriguing properties, and integration of such materials for potential device applications will necessarily invoke further reduction of their dimensionality. Using first-principles approaches, here we investigate the structural, electronic, and magnetic properties along the two different edges of zigzag MX2 (M = Mo, W; X = S, Se) nanoribbons. Along the M edges, we reveal a previously unrecognized but energetically strongly preferred (2 × 1) reconstruction pattern, which is universally operative for all the four systems (and possibly more), characterized by an elegant self-passivation mechanism through place exchanges of the outmost X and M edge atoms. In contrast, the X edges undergo a much milder (2 × 1) or (3 × 1) reconstruction for MoX2 or WX2, respectively. These contrasting structural preferences of the edges can be exploited for controlled fabrication of properly tailored transition metal dichalcogenide nanoribbons under nonequilibrium growth conditions. We further use the zigzag MoX2 nanoribbons to demonstrate that the Mo and X edges possess distinctly different electronic and magnetic properties, which are significant for catalytic and spintronic applications.

Semiconductor plasmonic nanolasers: current status and perspectives.

Scaling down semiconductor lasers in all three dimensions holds the key to the development of compact, low-threshold, and ultrafast coherent light sources, as well as integrated optoelectronic and plasmonic circuits. However, the minimum size of conventional semiconductor lasers utilizing dielectric cavity resonators (photonic cavities) is limited by the diffraction limit. To date, surface plasmon amplification by stimulated emission of radiation (spaser)-based plasmonic nanolaser is the only photon and plasmon-emitting device capable of this remarkable feat. Specifically, it has been experimentally demonstrated that the use of plasmonic cavities based on metal-insulator-semiconductor (MIS) nanostructures can indeed break the diffraction limit in all three dimensions. In this review, we present an updated overview of the current status for plasmonic nanolasers using the MIS configuration and other related metal-cladded semiconductor microlasers. In particular, by using composition-varied indium gallium nitride/gallium nitride core-shell nanorods, it is possible to realize all-color, single-mode nanolasers in the full visible wavelength range with ultralow continuous-wave (CW) lasing thresholds. The lasing action in these subdiffraction plasmonic cavities is achieved via a unique auto-tuning mechanism based on the property of weak size dependence inherent in plasmonic nanolasers. As for the choice of metals in the plasmonic structures, epitaxial silver films and giant colloidal silver crystals have been shown to be the superior constituent materials for plasmonic cavities due to their low plasmonic losses in the visible and near-infrared (NIR) spectral regions. In this review, we also provide some perspectives on the challenges and opportunities in this exciting new research frontier.

Probing Critical Point Energies of Transition Metal Dichalcogenides: Surprising Indirect Gap of Single Layer WSe2.

By using a comprehensive form of scanning tunneling spectroscopy, we have revealed detailed quasi-particle electronic structures in transition metal dichalcogenides, including the quasi-particle gaps, critical point energy locations, and their origins in the Brillouin zones. We show that single layer WSe2 surprisingly has an indirect quasi-particle gap with the conduction band minimum located at the Q-point (instead of K), albeit the two states are nearly degenerate. We have further observed rich quasi-particle electronic structures of transition metal dichalcogenides as a function of atomic structures and spin-orbit couplings. Such a local probe for detailed electronic structures in conduction and valence bands will be ideal to investigate how electronic structures of transition metal dichalcogenides are influenced by variations of local environment.