Van der Waals heterostructure polaritons with moiré-induced nonlinearity.

Controlling matter-light interactions with cavities is of fundamental importance in modern science and technology1. This is exemplified in the strong-coupling regime, where matter-light hybrid modes form, with properties that are controllable by optical-wavelength photons2,3. By contrast, matter excitations on the nanometre scale are harder to access. In two-dimensional van der Waals heterostructures, a tunable moiré lattice potential for electronic excitations may form4, enabling the generation of correlated electron gases in the lattice potentials5-9. Excitons confined in moiré lattices have also been reported10,11, but no cooperative effects have been observed and interactions with light have remained perturbative12-15. Here, by integrating MoSe2-WS2 heterobilayers in a microcavity, we establish cooperative coupling between moiré-lattice excitons and microcavity photons up to the temperature of liquid nitrogen, thereby integrating versatile control of both matter and light into one platform. The density dependence of the moiré polaritons reveals strong nonlinearity due to exciton blockade, suppressed exciton energy shift and suppressed excitation-induced dephasing, all of which are consistent with the quantum confined nature of the moiré excitons. Such a moiré polariton system combines strong nonlinearity and microscopic-scale tuning of matter excitations using cavity engineering and long-range light coherence, providing a platform with which to study collective phenomena from tunable arrays of quantum emitters.

Ultracompact Pseudowedge Plasmonic Lasers and Laser Arrays.

Concentrating light at the deep subwavelength scale by utilizing plasmonic effects has been reported in various optoelectronic devices with intriguing phenomena and functionality. Plasmonic waveguides with a planar structure exhibit a two-dimensional degree of freedom for the surface plasmon; the degree of freedom can be further reduced by utilizing metallic nanostructures or nanoparticles for surface plasmon resonance. Reduction leads to different lightwave confinement capabilities, which can be utilized to construct plasmonic nanolaser cavities. However, most theoretical and experimental research efforts have focused on planar surface plasmon polariton (SPP) nanolasers. In this study, we combined nanometallic structures intersecting with ZnO nanowires and realized the first laser emission based on pseudowedge SPP waveguides. Relative to current plasmonic nanolasers, the pseudowedge plasmonic lasers reported in our study exhibit extremely small mode volumes, high group indices, high spontaneous emission factors, and high Purell factors beneficial for the strong interaction between light and matter. Furthermore, we demonstrated that compact plasmonic laser arrays can be constructed, which could benefit integrated plasmonic circuits.

High-Operation-Temperature Plasmonic Nanolasers on Single-Crystalline Aluminum.

The recent development of plasmonics has overcome the optical diffraction limit and fostered the development of several important components including nanolasers, low-operation-power modulators, and high-speed detectors. In particular, the advent of surface-plasmon-polariton (SPP) nanolasers has enabled the development of coherent emitters approaching the nanoscale. SPP nanolasers widely adopted metal-insulator-semiconductor structures because the presence of an insulator can prevent large metal loss. However, the insulator is not necessary if permittivity combination of laser structures is properly designed. Here, we experimentally demonstrate a SPP nanolaser with a ZnO nanowire on the as-grown single-crystalline aluminum. The average lasing threshold of this simple structure is 20 MW/cm(2), which is four-times lower than that of structures with additional insulator layers. Furthermore, single-mode laser operation can be sustained at temperatures up to 353 K. Our study represents a major step toward the practical realization of SPP nanolasers.

Localized surface plasmon for enhanced lasing performance in solution-processed perovskites.

A promising method to promote the lasing performance of solution-processed organic-inorganic lead-halide perovskites has been demonstrated. With the adding Ag and PMMA thin films, the threshold excitation power for low-temperature lasing action in perovskites can be greatly reduced by over two orders of magnitude than that acquired in bare perovskite layers, ascribing to the strong exciton-plasmon coupling between the Ag and perovskite films. Also, the PMMA layer can be exploited to prevent the perovskite degradation from the hydrolysis in ambient environment, achieving long-lasting light-emitting performance. The advantages exhibited by the hybrid perovskite configuration would be very promising in making practical laser devices.

Cavity Floquet engineering.

Floquet engineering is a promising tool to manipulate quantum systems coherently. A well-known example is the optical Stark effect, which has been used for optical trapping of atoms and breaking time-reversal symmetry in solids. However, as a coherent nonlinear optical effect, Floquet engineering typically requires high field intensities obtained in ultrafast pulses, severely limiting its use. Here, we demonstrate using cavity engineering of the vacuum modes to achieve orders-of-magnitude enhancement of the effective Floquet field, enabling Floquet effects at an extremely low fluence of 450 photons/µm2. At higher fluences, the cavity-enhanced Floquet effects lead to 50 meV spin and valley splitting of WSe2 excitons, corresponding to an enormous time-reversal breaking, non-Maxwellian magnetic field of over 200 T. Utilizing such an optically controlled effective magnetic field, we demonstrate an ultrafast, picojoule chirality XOR gate. These results suggest that cavity-enhanced Floquet engineering may enable the creation of steady-state or quasi-equilibrium Floquet bands, strongly non-perturbative modifications of materials beyond the reach of other means, and application of Floquet engineering to a wide range of materials and applications.

Controllable Crystal Growth and Improved Photocatalytic Activity of Porous Bi2O3-Bi2S3 Composite Sheets.

Porous Bi2O3-Bi2S3 composite sheets were constructed through a combinational methodology of chemical bath deposition and hydrothermal reaction. The Na2S precursor concentration in the hydrothermal solution was varied to understand the correlation between the vulcanization degree and structure evolution of the porous Bi2O3-Bi2S3 composite sheets. The control of the etching rate of the Bi2O3 sheet template and the regrowth rate of Bi2S3 crystallites via suitable sulfide precursor concentration during the hydrothermal reaction utilizes the formation of porous Bi2O3-Bi2S3 sheets. Due to the presence of Bi2S3 crystallites and porous structure in the Bi2O3-Bi2S3 composites, the improved visible-light absorption ability and separation efficiency of photogenerated charge carriers are achieved. Furthermore, the as-synthesized Bi2O3-Bi2S3 composite sheets obtained from vulcanization with a 0.01M Na2S precursor display highly enhanced photocatalytic degradation toward methyl orange (MO) dyes compared with the pristine Bi2O3 and Bi2S3. The porous Bi2O3-Bi2S3 sheet system shows high surface active sites, fast transfer, high-efficiency separation of photoinduced charge carriers, and enhanced redox capacity concerning their constituent counterparts. This study affords a promising approach to constructing Bi2O3-based Z-scheme composites with a suitable microstructure and Bi2O3/Bi2S3 phase ratio for photoactive device applications.

Hemispherical Cesium Lead Bromide Perovskite Single-Mode Microlasers with High-Quality Factors and Strong Purcell Enhancement.

We realized a single-mode laser with an ultra-high quality factor in individual cesium lead bromide (CsPbBr3) perovskite micro-hemispheres fabricated by chemical vapor deposition. A series of lasing property analysis based on cavity size was reported under this material system. Due to good optical confinement capability of the whispering gallery resonant cavity and high optical gain of CsPbBr3 perovskite micro-hemispheres, single-mode lasing behavior was achieved with an ultra-high quality factor as large as 11,460 at room temperature. To study in detail the physical effects between lasing threshold and cavity, a set of cavity size dependence photoluminescence analyses were performed. We found that the lasing threshold increases while the cavity size decreases. Time-resolved PL analysis was conducted to confirm the relation between cavity size and lasing threshold. The larger cavity stands for longer PL lifetime and indicates easier-to-achieve carrier population inversion. Strong Purcell enhancement could be further investigated by the spontaneous emission coupling factor ß and internal quantum efficiency as a function of cavity size. A high ß-factor of 0.37 could be obtained from a 2.2 µm diameter hemisphere microcavity and a high Purcell factor of 14 in a 1.9 µm diameter hemisphere microcavity showing strong Purcell enhancement effect in our system.

One- and Two-Photon Excited Photoluminescence and Suppression of Thermal Quenching of CsSnBr3 Microsquare and Micropyramid.

Thermal photoluminescence (PL) quenching is fundamentally important for perovskite optoelectronic applications. Herein, we investigated PL characteristics of CsSnBr3 microsquares and micropyramids synthesized by chemical vapor deposition (CVD) and their PL quenching behavior at high temperature. These microstructures have favorable PL performances in ambient atmosphere. Under two-photon excitation, we observed whispering gallery modes (WGMs) in microsquares and amplified spontaneous emission (ASE) in micropyramids. Reversible PL losses due to thermal effect were observed for both samples. Monotonic blue shifts in PL emission upon temperature increase suggest a band gap widening associated with an emphanisis effect. Temperature-dependent spectral line width analysis reveals that a line width broadening is attributed to the dominant electron-longitudinal optical phonon interaction. The estimated activation energy of thermally assisted nonradiative recombination for CsSnBr3 microsquares and micropyramids is over 310 meV by the Arrhenius equation, which is higher than CsPbBr3. These results prove that CsSnBr3 exhibits better thermal stability than Pb-based perovskites.

Improved photoelectrode performance of chemical solution-derived Bi2O3 crystals via manipulation of crystal characterization.

Three-dimensional Bi2O3 crystals with various morphologies were successfully synthesized on F-doped tin oxide substrates with and without homoseed layers via chemical bath deposition (CBD) routes. The structural analysis reveals that control of the pH value of the reaction solution resulted in as-grown Bi2O3 crystals with nanosheet and plate morphologies. A lower pH value of the reaction solution engendered formation of a porous sheet-like morphology of Bi2O3; by contrast, a higher pH value of the reaction solution is favorable for formation of solid Bi2O3 plates on the substrates. Furthermore, a sputter coated Bi2O3 seed layer with dual α- and ß-Bi2O3 phases plays an important role in the CBD-derived Bi2O3 crystallographic structures. The Bi2O3 crystals formed via CBD processes without a sputter coated Bi2O3 homoseed layer demonstrated a high purity in ß-Bi2O3 phase; those grown with a homoseed layer exhibited a dual α/ß phase. The photoactive performance results show that construction of an α/ß-Bi2O3 homojunction in the CBD-derived Bi2O3 crystals substantially improved their photoactive performance. Comparatively, the porous Bi2O3 nanosheets with a dual α/ß-Bi2O3 phase demonstrated the highest photoactive performance among various Bi2O3 crystals in this study. The superior photoactivity of the porous α/ß-Bi2O3 nanosheets herein is attributed to their high light absorption capacity and photoinduced charge separation efficiency. The experimental results in this study provide a promising approach to design CBD-derived Bi2O3 crystals with desirable photoelectric conversion functions via facile morphology control and seed layer crystal engineering.

Surface roughness effects on aluminium-based ultraviolet plasmonic nanolasers.

We systematically investigate the effects of surface roughness on the characteristics of ultraviolet zinc oxide plasmonic nanolasers fabricated on aluminium films with two different degrees of surface roughness. We demonstrate that the effective dielectric functions of aluminium interfaces with distinct roughness can be analysed from reflectivity measurements. By considering the scattering losses, including Rayleigh scattering, electron scattering, and grain boundary scattering, we adopt the modified Drude-Lorentz model to describe the scattering effect caused by surface roughness and obtain the effective dielectric functions of different Al samples. The sample with higher surface roughness induces more electron scattering and light scattering for SPP modes, leading to a higher threshold gain for the plasmonic nanolaser. By considering the pumping efficiency, our theoretical analysis shows that diminishing the detrimental optical losses caused by the roughness of the metallic interface could effectively lower (~33.1%) the pumping threshold of the plasmonic nanolasers, which is consistent with the experimental results.

Crossover from polariton lasing to exciton lasing in a strongly coupled ZnO microcavity.

Unlike conventional photon lasing, in which the threshold is limited by the population inversion of the electron-hole plasma, the exciton lasing generated by exciton-exciton scattering and the polariton lasing generated by dynamical condensates have received considerable attention in recent years because of the sub-Mott density and low-threshold operation. This paper presents a novel approach to generate both exciton and polariton lasing in a strongly coupled microcavity (MC) and determine the critical driving requirements for simultaneously triggering these two lasing operation in temperature <140 K and large negative polariton-exciton offset (<-133 meV) conditions. In addition, the corresponding lasing behaviors, such as threshold energy, linewidth, phase diagram, and angular dispersion are verified. The results afford a basis from which to understand the complicated lasing mechanisms in strongly coupled MCs and verify a new method with which to trigger dual laser emission based on exciton and polariton.

Controllable lasing performance in solution-processed organic-inorganic hybrid perovskites.

Solution-processed organic-inorganic perovskites are fascinating due to their remarkable photo-conversion efficiency and great potential in the cost-effective, versatile and large-scale manufacturing of optoelectronic devices. In this paper, we demonstrate that the perovskite nanocrystal sizes can be simply controlled by manipulating the precursor solution concentrations in a two-step sequential deposition process, thus achieving the feasible tunability of excitonic properties and lasing performance in hybrid metal-halide perovskites. The lasing threshold is at around 230 µJ cm-2 in this solution-processed organic-inorganic lead-halide material, which is comparable to the colloidal quantum dot lasers. The efficient stimulated emission originates from the multiple random scattering provided by the micro-meter scale rugged morphology and polycrystalline grain boundaries. Thus the excitonic properties in perovskites exhibit high correlation with the formed morphology of the perovskite nanocrystals. Compared to the conventional lasers normally serving as a coherent light source, the perovskite random lasers are promising in making low-cost thin-film lasing devices for flexible and speckle-free imaging applications.

Single-crystalline aluminum film for ultraviolet plasmonic nanolasers.

Significant advances have been made in the development of plasmonic devices in the past decade. Plasmonic nanolasers, which display interesting properties, have come to play an important role in biomedicine, chemical sensors, information technology, and optical integrated circuits. However, nanoscale plasmonic devices, particularly those operating in the ultraviolet regime, are extremely sensitive to the metal and interface quality. Thus, these factors have a significant bearing on the development of ultraviolet plasmonic devices. Here, by addressing these material-related issues, we demonstrate a low-threshold, high-characteristic-temperature metal-oxide-semiconductor ZnO nanolaser that operates at room temperature. The template for the ZnO nanowires consists of a flat single-crystalline Al film grown by molecular beam epitaxy and an ultrasmooth Al2O3 spacer layer synthesized by atomic layer deposition. By effectively reducing the surface plasmon scattering and metal intrinsic absorption losses, the high-quality metal film and the sharp interfaces formed between the layers boost the device performance. This work should pave the way for the use of ultraviolet plasmonic nanolasers and related devices in a wider range of applications.

ZnO-Based Microcavities Sculpted by Focus Ion Beam Milling.

We reported an easy fabrication method to realize ZnO-based microcavities with various cavity shapes by focused ion beam (FIB) milling. The optical characteristics of different shaped microcavities have been systematically carried out and analyzed. Through comprehensive studies of cathodoluminescence and photoluminescence spectra, the whispering gallery mode (WGM) was observed in different shaped microcavities. Up further increasing excitation, the lasing action was dominated by these WGMs and matched very well to the simulated results. Our experiment shows that ZnO microcavities with different shapes can be made with high quality by FIB milling for specific applications of microlight sources and optical devices.

Ultrastrong Mode Confinement in ZnO Surface Plasmon Nanolasers.

Nanolasers with an ultracompact footprint can provide high-intensity coherent light, which can be potentially applied to high-capacity signal processing, biosensing, and subwavelength imaging. Among various nanolasers, those with cavities surrounded by metals have been shown to have superior light emission properties because of the surface plasmon effect that provides enhanced field confinement capability and enables exotic light-matter interaction. In this study, we demonstrated a robust ultraviolet ZnO nanolaser that can operate at room temperature by using silver to dramatically shrink the mode volume. The nanolaser shows several distinct features including an extremely small mode volume, a large Purcell factor, and a slow group velocity, which ensures strong interaction with the exciton in the nanowire.