Single-layer direct band gap semiconductors such as transition metal dichalcogenides are quite attractive for a wide range of electronics, photonics, and optoelectronics applications. Their monolayer ...thickness provides significant advantages in many applications such as field-effect transistors for high-performance electronics, sensor/detector applications, and flexible electronics. However, for optoelectronics and photonics applications, inherent monolayer thickness poses a significant challenge for the interaction of light with the material, which therefore results in poor light emission and absorption behavior. Here, we demonstrate enhanced light emission from large-area monolayer MoS2 using plasmonic silver nanodisc arrays, where enhanced photoluminescence up to 12-times has been measured. Observed phenomena stem from the fact that plasmonic resonance couples to both excitation and emission fields and thus boosts the light–matter interaction at the nanoscale. Reported results allow us to engineer light–matter interactions in two-dimensional materials and could enable highly efficient photodetectors, sensors, and photovoltaic devices, where photon absorption and emission efficiency highly dictate the device performance.
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.Scanning tunnelling spectroscopy and ab initio simulations reveal buckling reconstruction and in-plane strain redistribution in WSe2/WS2 moiré heterostructures.
Abstract
Heterobilayers of transition metal dichalcogenides (TMDCs) can form a moiré superlattice with flat minibands, which enables strong electron interaction and leads to various fascinating ...correlated states. These heterobilayers also host interlayer excitons in a type-II band alignment, in which optically excited electrons and holes reside on different layers but remain bound by the Coulomb interaction. Here we explore the unique setting of interlayer excitons interacting with strongly correlated electrons, and we show that the photoluminescence (PL) of interlayer excitons sensitively signals the onset of various correlated insulating states as the band filling is varied. When the system is in one of such states, the PL of interlayer excitons is relatively amplified at increased optical excitation power due to reduced mobility, and the valley polarization of interlayer excitons is enhanced. The moiré superlattice of the TMDC heterobilayer presents an exciting platform to engineer interlayer excitons through the periodic correlated electron states.
Abstract
Tungsten-based monolayer transition metal dichalcogenides host a long-lived “dark” exciton, an electron-hole pair in a spin-triplet configuration. The long lifetime and unique spin ...properties of the dark exciton provide exciting opportunities to explore light-matter interactions beyond electric dipole transitions. Here we demonstrate that the coupling of the dark exciton and an optically silent chiral phonon enables the intrinsic photoluminescence of the dark-exciton replica in monolayer WSe
2
. Gate and magnetic-field dependent PL measurements unveil a circularly-polarized replica peak located below the dark exciton by 21.6 meV, equal to E″ phonon energy from Se vibrations. First-principles calculations show that the exciton-phonon interaction selectively couples the spin-forbidden dark exciton to the intravalley spin-allowed bright exciton, permitting the simultaneous emission of a chiral phonon and a circularly-polarized photon. Our discovery and understanding of the phonon replica reveals a chirality dictated emission channel of the phonons and photons, unveiling a new route of manipulating valley-spin.
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, miniDirac 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 transitionmetal dichalcogenides.
Van der Waals heterostructures have recently emerged as a new class of materials, where quantum coupling between stacked atomically thin two-dimensional layers, including graphene, hexagonal-boron ...nitride and transition-metal dichalcogenides (MX2), give rise to fascinating new phenomena. MX2 heterostructures are particularly exciting for novel optoelectronic and photovoltaic applications, because two-dimensional MX2 monolayers can have an optical bandgap in the near-infrared to visible spectral range and exhibit extremely strong light-matter interactions. Theory predicts that many stacked MX2 heterostructures form type II semiconductor heterojunctions that facilitate efficient electron-hole separation for light detection and harvesting. Here, we report the first experimental observation of ultrafast charge transfer in photoexcited MoS2/WS2 heterostructures using both photoluminescence mapping and femtosecond pump-probe spectroscopy. We show that hole transfer from the MoS2 layer to the WS2 layer takes place within 50 fs after optical excitation, a remarkable rate for van der Waals coupled two-dimensional layers. Such ultrafast charge transfer in van der Waals heterostructures can enable novel two-dimensional devices for optoelectronics and light harvesting.
Tracking the spin-valley currentTaking advantage of the electron's spin and valley degrees of freedom requires a method for generating currents of carriers that have a particular spin or come from a ...particular valley in the electronic structure. Jin et al. used a heterostructure made out of adjacent layers of WSe2 and WS2 to create a spin-valley diffusion current without applying an external electric field. Instead, they used circularly polarized laser light to initiate the diffusion and a second laser pulse to image the propagation of the carriers. With long lifetimes and diffusion lengths, the method may be of practical use in future valleytronic devices.Science, this issue p. 893Transition metal dichalcogenide (TMDC) materials are promising for spintronic and valleytronic applications because valley-polarized excitations can be generated and manipulated with circularly polarized photons and the valley and spin degrees of freedom are locked by strong spin-orbital interactions. In this study we demonstrate efficient generation of a pure and locked spin-valley diffusion current in tungsten disulfide (WS2)–tungsten diselenide (WSe2) heterostructures without any driving electric field. We imaged the propagation of valley current in real time and space by pump-probe spectroscopy. The valley current in the heterostructures can live for more than 20 microseconds and propagate over 20 micrometers; both the lifetime and the diffusion length can be controlled through electrostatic gating. The high-efficiency and electric-field–free generation of a locked spin-valley current in TMDC heterostructures holds promise for applications in spin and valley devices.
Van der Waals （vdW） heterojunctions are equipped to avert dangling bonds due to weak, inter-layer vdW force, and ensure strong in-plane covalent bonding for two-dimensional layered structures. We ...fabricated four heterojunctions devices of different layers based on p-type distorted 1T-MX2 ReSe2 and n-type hexagonal MoS2 nanoflakes, and measured their electronic and optoelectronic properties. The device showed a high rectification coefficient of 500 for the diode, a high ON/OFF ratio and higher electron mobility for the field-effect transistor （FET） compared with the individual components, and a high current responsivity （Rλ） and external quantum efficiency （EQE） of 6.75 A/W and 1,266%, respectively, for the photodetector.
The emergence of two-dimensional crystals has revolutionized modern solid-state physics. From a fundamental point of view, the enhancement of charge carrier correlations has sparked much research ...activity in the transport and quantum optics communities. One of the most intriguing effects, in this regard, is the bosonic condensation and spontaneous coherence of many-particle complexes. Here we find compelling evidence of bosonic condensation of exciton-polaritons emerging from an atomically thin crystal of MoSe
embedded in a dielectric microcavity under optical pumping at cryogenic temperatures. The formation of the condensate manifests itself in a sudden increase of luminescence intensity in a threshold-like manner, and a notable spin-polarizability in an externally applied magnetic field. Spatial coherence is mapped out via highly resolved real-space interferometry, revealing a spatially extended condensate. Our device represents a decisive step towards the implementation of coherent light-sources based on atomically thin crystals, as well as non-linear, valleytronic coherent devices.
Layered semiconductors based on transition-metal chalcogenides usually cross from indirect bandgap in the bulk limit over to direct bandgap in the quantum (2D) limit. Such a crossover can be achieved ...by peeling off a multilayer sample to a single layer. For exploration of physical behavior and device applications, it is much desired to reversibly modulate such crossover in a multilayer sample. Here we demonstrate that, in a few-layer sample where the indirect bandgap and direct bandgap are nearly degenerate, the temperature rise can effectively drive the system toward the 2D limit by thermally decoupling neighboring layers via interlayer thermal expansion. Such a situation is realized in few-layer MoSe2, which shows stark contrast from the well-explored MoS2 where the indirect and direct bandgaps are far from degenerate. Photoluminescence of few-layer MoSe2 is much enhanced with the temperature rise, much like the way that the photoluminescence is enhanced due to the bandgap crossover going from the bulk to the quantum limit, offering potential applications involving external modulation of optical properties in 2D semiconductors. The direct bandgap of MoSe2, identified at 1.55 eV, may also promise applications in energy conversion involving solar spectrum, as it is close to the optimal bandgap value of single-junction solar cells and photoelechemical devices.
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