Room-Temperature Geometrical Circular Photocurrent in Few-Layer MoS2.

Valleytronics, i.e., the manipulation of the valley degree of freedom, offers a promising path for energy-efficient electronics. One of the key milestones in this field is the room-temperature manipulation of the valley information in thick-layered material. Using scanning photocurrent microscopy, we achieve this milestone by observing a geometrically dependent circular photocurrent in a few-layer molybdenum disulfide (MoS2) under normal incidence. Such an observation shows that the system symmetry is lower than that of bulk MoS2 material, preserving the optical chirality-valley correspondence. Moreover, the circular photocurrent polarity can be reversed by applying electrical bias. We propose a model where the observed photocurrent results from the symmetry breaking and the built-in field at the electrode-sample interface. Our results show that the valley information is still retained even in thick-layered MoS2 at room temperature and opens up new opportunities for exploiting the valley index through interface engineering in multilayer valleytronics devices.

Interlayer donor-acceptor pair excitons in MoSe2/WSe2 moiré heterobilayer.

Localized interlayer excitons (LIXs) in two-dimensional moiré superlattices exhibit sharp and dense emission peaks, making them promising as highly tunable single-photon sources. However, the fundamental nature of these LIXs is still elusive. Here, we show the donor-acceptor pair (DAP) mechanism as one of the origins of these excitonic peaks. Numerical simulation results of the DAP model agree with the experimental photoluminescence spectra of LIX in the moiré MoSe2/WSe2 heterobilayer. In particular, we find that the emission energy-lifetime correlation and the nonmonotonic power dependence of the lifetime agree well with the DAP IX model. Our results provide insight into the physical mechanism of LIX formation in moiré heterostructures and pave new directions for engineering interlayer exciton properties in moiré superlattices.

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.

Magnetically Tunable Spontaneous Superradiance from Mesoscopic Perovskite Emitter Clusters.

Perovskite emitters are promising materials as next-generation optical sources due to their low fabrication cost and high quantum yield. In particular, the superradiant emission from a few coherently coupled perovskite emitters can be used to produce a bright entangled photon source. Here, we report the observation of superradiance from mesoscopic (<55) CsPbBr3 perovskite emitters, which have a much smaller ensemble size than the previously reported results (>106 emitters). The superradiance is spontaneously generated by off-resonance excitation and detected by time-resolved photoluminescence and second-order photon correlation measurements. We observed a remarkable magnetic tunability of the superradiant photon bunching, indicating a magnetic field-induced decoherence process. The experimental results can be well explained using a theoretical framework based on the microscopic master equation. Our findings shed light on the superradiance mechanism in perovskite emitters and enable low-cost quantum light sources based on perovskite.

Dual-Gate All-Electrical Valleytronic Transistors.

The development of integrated circuits (ICs) based on a complementary metal-oxide-semiconductor through transistor scaling has reached the technology bottleneck; thus, alternative approaches from new physical mechanisms are highly demanded. Valleytronics in two-dimensional (2D) material systems has recently emerged as a strong candidate, which utilizes the valley degree of freedom to process information for electronic applications. However, for all-electrical valleytronic transistors, very low room-temperature "valley on-off" ratios (around 10) have been reported so far, which seriously limits their practical applications. In this work, we successfully illustrated both n- and p-type valleytronic transistor performances in monolayer MoS2 and WSe2 devices, with measured "valley on-off" ratios improved up to 3 orders of magnitude greater compared to previous reports. Our work shows a promising way for the electrically controllable manipulation of valley degree of freedom toward practical device applications.

Signature of Cascade Transitions between Interlayer Excitons in a Moiré Superlattice.

A moiré superlattice in transition metal dichalcogenides heterostructure provides an exciting platform for studying strongly correlated electronics and excitonic physics, such as multiple interlayer exciton (IX) energy bands. However, the correlations between these IXs remain elusive. Here, we demonstrate the cascade transitions between IXs in a moiré superlattice by performing energy- and time-resolved photoluminescence measurements in the MoS_{2}/WSe_{2} heterostructure. Furthermore, we show that the lower-energy IX can be excited to higher-energy ones, facilitating IX population inversion. Our finding of cascade transitions between IXs contributes to the fundamental understanding of the IX dynamics in moiré superlattices and may have important applications, such as in exciton condensate, quantum information protocols, and quantum cascade lasers.

Layer-engineered interlayer excitons.

Photoluminescence (PL) from excitons serves as a powerful tool to characterize the optoelectronic property and band structure of semiconductors, especially for atomically thin two-dimensional transition metal dichalcogenide (TMD) materials. However, PL quenches quickly when the thickness of TMD materials increases from monolayer to a few layers, due to the change from direct to indirect band transition. Here, we show that PL can be recovered by engineering multilayer heterostructures, with the band transition reserved to be a direct type. We report emission from layer-engineered interlayer excitons from these multilayer heterostructures. Moreover, as desired for valleytronics devices, the lifetime, valley polarization, and valley lifetime of the generated interlayer excitons can all be substantially improved as compared with that in the monolayer-monolayer heterostructure. Our results pave the way for controlling the properties of interlayer excitons by layer engineering.

Room temperature nanocavity laser with interlayer excitons in 2D heterostructures.

Atomically thin layered two-dimensional (2D) materials have provided a rich library for both fundamental research and device applications. Bandgap engineering and controlled material response can be achieved from artificial heterostructures. Recently, excitonic lasers have been reported using transition metal dichalcogenides; however, the emission is still the intrinsic energy bandgap of the monolayers. Here, we report a room temperature interlayer exciton laser with MoS2/WSe2 heterostructures. The onset of lasing was identified by the distinct kink in the "L-L" curve and the noticeable spectral linewidth collapse. Different from visible emission of intralayer excitons in monolayer components, our laser works in the infrared range, which is fully compatible with the well-established technologies in silicon photonics. Long lifetime of interlayer excitons relaxes the requirement of the cavity quality factor by orders of magnitude. Room temperature interlayer exciton lasers might open new perspectives for developing coherent light sources with tailored optical properties on silicon photonics platforms.

Direct Photoluminescence Probing of Ferromagnetism in Monolayer Two-Dimensional CrBr3.

Atomically thin magnets are the key element to build up spintronics based on two-dimensional materials. The surface nature of two-dimensional ferromagnet opens up opportunities to improve the device performance efficiently. Here, we report the intrinsic ferromagnetism in atomically thin monolayer CrBr3, directly probed by polarization resolved magneto-photoluminescence. The spontaneous magnetization persists in monolayer CrBr3 with a Curie temperature of 34 K. The development of magnons by the thermal excitation is in line with the spin-wave theory. We attribute the layer-number-dependent hysteresis loops in thick layers to the magnetic domain structures. As a stable monolayer material in air, CrBr3 provides a convenient platform for fundamental physics and pushes the potential applications of the two-dimensional ferromagnetism.

Theoretical Prediction of Chiral 3D Hybrid Organic-Inorganic Perovskites.

Hybrid organic-inorganic perovskites (HOIPs), in particular 3D HOIPs, have demonstrated remarkable properties, including ultralong charge-carrier diffusion lengths, high dielectric constants, low trap densities, tunable absorption and emission wavelengths, strong spin-orbit coupling, and large Rashba splitting. These superior properties have generated intensive research interest in HOIPs for high-performance optoelectronics and spintronics. Here, 3D hybrid organic-inorganic perovskites that implant chirality through introducing the chiral methylammonium cation are demonstrated. Based on structural optimization, phonon spectra, formation energy, and ab initio molecular dynamics simulations, it is found that the chirality of the chiral cations can be successfully transferred to the framework of 3D HOIPs, and the resulting 3D chiral HOIPs are both kinetically and thermodynamically stable. Combining chirality with the impressive optical, electrical, and spintronic properties of 3D perovskites, 3D chiral perovskites is of great interest in the fields of piezoelectricity, pyroelectricity, ferroelectricity, topological quantum engineering, circularly polarized optoelectronics, and spintronics.

Bright room temperature single photon source at telecom range in cubic silicon carbide.

Single-photon emitters (SPEs) play an important role in a number of quantum information tasks such as quantum key distributions. In these protocols, telecom wavelength photons are desired due to their low transmission loss in optical fibers. In this paper, we present a study of bright single-photon emitters in cubic silicon carbide (3C-SiC) emitting in the telecom range. We find that these emitters are photostable and bright at room temperature with a count rate of ~ MHz. Altogether with the fact that SiC is a growth and fabrication-friendly material, our result may be relevant for future applications in quantum communication technology.

Room temperature solid-state quantum emitters in the telecom range.

On-demand, single-photon emitters (SPEs) play a key role across a broad range of quantum technologies. In quantum networks and quantum key distribution protocols, where photons are used as flying qubits, telecom wavelength operation is preferred because of the reduced fiber loss. However, despite the tremendous efforts to develop various triggered SPE platforms, a robust source of triggered SPEs operating at room temperature and the telecom wavelength is still missing. We report a triggered, optically stable, room temperature solid-state SPE operating at telecom wavelengths. The emitters exhibit high photon purity (~5% multiphoton events) and a record-high brightness of ~1.5 MHz. The emission is attributed to localized defects in a gallium nitride (GaN) crystal. The high-performance SPEs embedded in a technologically mature semiconductor are promising for on-chip quantum simulators and practical quantum communication technologies.

Microsecond dark-exciton valley polarization memory in two-dimensional heterostructures.

Transition metal dichalcogenides have valley degree of freedom, which features optical selection rule and spin-valley locking, making them promising for valleytronics devices and quantum computation. For either application, a long valley polarization lifetime is crucial. Previous results showed that it is around picosecond in monolayer excitons, nanosecond for local excitons and tens of nanosecond for interlayer excitons. Here we show that the dark excitons in two-dimensional heterostructures provide a microsecond valley polarization memory thanks to the magnetic field induced suppression of valley mixing. The lifetime of the dark excitons shows magnetic field and temperature dependence. The long lifetime and valley polarization lifetime of the dark exciton in two-dimensional heterostructures make them promising for long-distance exciton transport and macroscopic quantum state generations.

Zeeman splitting via spin-valley-layer coupling in bilayer MoTe2.

Atomically thin monolayer transition metal dichalcogenides possess coupling of spin and valley degrees of freedom. The chirality is locked to identical valleys as a consequence of spin-orbit coupling and inversion symmetry breaking, leading to a valley analog of the Zeeman effect in presence of an out-of-plane magnetic field. Owing to the inversion symmetry in bilayers, the photoluminescence helicity should no longer be locked to the valleys. Here we show that the Zeeman splitting, however, persists in 2H-MoTe2 bilayers, as a result of an additional degree of freedom, namely the layer pseudospin, and spin-valley-layer locking. Unlike monolayers, the Zeeman splitting in bilayers occurs without lifting valley degeneracy. The degree of circularly polarized photoluminescence is tuned with magnetic field from -37% to 37%. Our results demonstrate the control of degree of freedom in bilayer with magnetic field, which makes bilayer a promising platform for spin-valley quantum gates based on magnetoelectric effects.Monolayer transition metal dichalcogenides host a valley splitting in magnetic field analogous to the Zeeman effect. Here, the authors report that the Zeeman splitting still persists in bilayers of MoTe2 without lifting the valley degeneracy, due to spin-valley-layer coupling.

Coherent control of a strongly driven silicon vacancy optical transition in diamond.

The ability to prepare, optically read out and coherently control single quantum states is a key requirement for quantum information processing. Optically active solid-state emitters have emerged as promising candidates with their prospects for on-chip integration as quantum nodes and sources of coherent photons connecting these nodes. Under a strongly driving resonant laser field, such quantum emitters can exhibit quantum behaviour such as Autler-Townes splitting and the Mollow triplet spectrum. Here we demonstrate coherent control of a strongly driven optical transition in silicon vacancy centre in diamond. Rapid optical detection of photons enabled the observation of time-resolved coherent Rabi oscillations and the Mollow triplet spectrum. Detection with a probing transition further confirmed Autler-Townes splitting generated by a strong laser field. The coherence time of the emitted photons is comparable to its lifetime and robust under a very strong driving field, which is promising for the generation of indistinguishable photons.