Exciton polariton condensation from bound states in the continuum at room temperature.

Exciton-polaritons (polaritons) resulting from the strong exciton-photon interaction stimulates the development of novel low-threshold coherent light sources to circumvent the ever-increasing energy demands of optical communications1-3. Polaritons from bound states in the continuum (BICs) are promising for Bose-Einstein condensation owing to their theoretically infinite quality factors, which provide prolonged lifetimes and benefit the polariton accumulations4-7. However, BIC polariton condensation remains limited to cryogenic temperatures ascribed to the small exciton binding energies of conventional material platforms. Herein, we demonstrated room-temperature BIC polariton condensation in perovskite photonic crystal lattices. BIC polariton condensation was demonstrated at the vicinity of the saddle point of polariton dispersion that generates directional vortex beam emission with long-range coherence. We also explore the peculiar switching effect among the miniaturized BIC polariton modes through effective polariton-polariton scattering. Our work paves the way for the practical implementation of BIC polariton condensates for integrated photonic and topological circuits.

Giant Out-of-Plane Exciton Emission Enhancement in Two-Dimensional Indium Selenide via a Plasmonic Nanocavity.

Out-of-plane (OP) exciton-based emitters in two-dimensional semiconductor materials are attractive candidates for novel photonic applications, such as radially polarized sources, integrated photonic chips, and quantum communications. However, their low quantum efficiency resulting from forbidden transitions limits their practicality. In this work, we achieve a giant enhancement of up to 34000 for OP exciton emission in indium selenide (InSe) via a designed Ag nanocube-over-Au film plasmonic nanocavity. The large photoluminescence enhancement factor (PLEF) is attributed to the induced OP local electric field (Ez) within the nanocavity, which facilitates effective OP exciton-plasmon interaction and subsequent tremendous enhancement. Moreover, the nanoantenna effect resulting from the effective interaction improves the directivity of spontaneous radiation. Our results not only reveal an effective photoluminescence enhancement approach for OP excitons but also present an avenue for designing on-chip photonic devices with an OP dipole orientation.

On-chip integrated exceptional surface microlaser.

The on-chip integrated visible microlaser is a core unit of high-speed visible-light communication with huge bandwidth resources, which needs robustness against fabrication errors, compressible linewidth, reducible threshold, and in-plane emission. However, until now, it has been a great challenge to meet these requirements simultaneously. Here, we report a scalable strategy to realize a robust on-chip integrated visible microlaser with further improved lasing performances enabled by the increased orders (n) of exceptional surfaces, and experimentally verify the strategy by demonstrating the performances of a second-order exceptional surface-tailored microlaser. We further prove the potential application of the strategy by discussing an exceptional surface-tailored topological microlaser with unique performances. This work lays a foundation for further development of on-chip integrated high-speed visible-light communication and processing systems, provides a platform for the fundamental study of non-Hermitian photonics, and proposes a feasible method of joint research for non-Hermitian photonics with nonlinear optics and topological photonics.

Edge Raman enhancement at layered PbI2platelets induced by laser waveguide effect.

As a two-dimensional (2D) layered semiconductor, lead iodide (PbI2) has been widely used in optoelectronics owing to its unique crystal structure and distinctive optical and electrical properties. A comprehensive understanding of its optical performance is essential for further application and progress. Here, we synthesized regularly shaped PbI2platelets using the chemical vapor deposition method. Raman scattering spectroscopy of PbI2platelets was predominantly enhanced when the laser radiated at the edge according to Raman mapping spectroscopy. Combining the outcome of polarized Raman scattering spectroscopy and finite-difference time domain simulation analysis, the Raman enhancement was proven to be the consequence of the enhancement effects inherent to the high refractive index contrast waveguide, which is naturally formed in well-defined PbI2platelets. Because of the enlarged excited area determined by the increased propagation length of the laser in the PbI2platelet formed waveguide, the total Raman enhancements are acquired rather than a localized point enhancement. Finally, the Raman enhancement factor is directly related to the thickness of the PbI2platelet, which further confirms the waveguide-enhanced edge Raman. Our investigation of the optical properties of PbI2platelets offers reference for potential 2D layered-related optoelectronic applications.

Large-Scale Thin CsPbBr3 Single-Crystal Film Grown on Sapphire via Chemical Vapor Deposition: Toward Laser Array Application.

Single-crystal perovskites with excellent photophysical properties are considered to be ideal materials for optoelectronic devices, such as lasers, light-emitting diodes and photodetectors. However, the growth of large-scale perovskite single-crystal films (SCFs) with high optical gain by vapor-phase epitaxy remains challenging. Herein, we demonstrated a facile method to fabricate large-scale thin CsPbBr3 SCFs (∼300 nm) on the c-plane sapphire substrate. High temperature is found to be the key parameter to control low reactant concentration and sufficient surface diffusion length for the growth of continuous CsPbBr3 SCFs. Through the comprehensive study of the carrier dynamics, we clarify that the trapped-related exciton recombination has the main effect under low carrier density, while the recombination of excitons and free carriers coexist until free carriers plays the dominate role with increasing carrier density. Furthermore, an extremely low-threshold (∼8 µJ cm-2) amplified spontaneous emission was achieved at room temperature due to the high optical gain up to 1255 cm-1 at a pump power of 20 times threshold (∼20 Pth). A microdisk array was prepared using a focused ion beam etching method, and a single-mode laser was achieved on a 3 µm diameter disk with the threshold of 1.6 µJ cm-2. Our experimental results not only present a versatile method to fabricate large-scale SCFs of CsPbBr3 but also supply an arena to boost the optoelectronic applications of CsPbBr3 with high performance.

Efficient Quasi-Two-Dimensional Perovskite Light-Emitting Diodes with Improved Multiple Quantum Well Structure.

Quasi-two-dimensional (quasi-2D) perovskites with a multiple quantum well structure can enhance the exciton binding energy and controllable quantum confine effect, which are attractive materials for efficient perovskite light-emitting diodes (PeLEDs). However, the multiphase mixtures contained in these materials would cause nonradiative recombination at the perovskite film surface. Here, a facile solution surface treatment is adopted to improve the multiple quantum well structure of the quasi-2D perovskite emitting layer, which can reduce the influence of defectinduced nonradiative recombination and the electric-field-induced dissociation of excitons for the PeLEDs. The improved multiple quantum well structure is verified by UV absorption spectra and temperature-dependent photoluminescence spectra measurements. The photoluminescence quantum yield of the quasi-2D perovskite film with surface treatment has been approximately increased by 200%. Meanwhile, the electroluminescence device achieves a current efficiency of 45.9 cd/A.

Lasing from Mechanically Exfoliated 2D Homologous Ruddlesden-Popper Perovskite Engineered by Inorganic Layer Thickness.

2D Ruddlesden-Popper perovskites (RPPs) have aroused growing attention in light harvesting and emission applications owing to their high environmental stability. Recently, coherent light emission of RPPs was reported, however mostly from inhomologous thin films that involve cascade intercompositional energy transfer. Lasing and fundamental understanding of intrinsic laser dynamics in homologous RPPs free from intercompositional energy transfer is still inadequate. Herein, the lasing and loss mechanisms of homologous 2D (BA)2 (MA)n -1 Pbn I3 n +1 RPP thin flakes mechanically exfoliated from the bulk crystal are reported. Multicolor lasing is achieved from the large-n RPPs (n ≥ 3) in the spectral range of 620-680 nm but not from small-n RPPs (n ≤ 2) even down to 78 K. With decreasing n, the lasing threshold increases significantly and the characteristic temperature decreases as 49, 25, and 20 K for n = 5, 4, and 3, respectively. The n-engineered lasing behaviors are attributed to the stronger Auger recombination and exciton-phonon interaction as a result of the enhanced quantum confinement in the smaller-n perovskites. These results not only advance the fundamental understanding of loss mechanisms in both inhomologous and homologous RPP lasers but also provide insights into developing low-threshold, substrate-free, and multicolor 2D semiconductor microlasers.

Vapor-Phase Incommensurate Heteroepitaxy of Oriented Single-Crystal CsPbBr3 on GaN: Toward Integrated Optoelectronic Applications.

Integrating metallic halide perovskites with established modern semiconductor technology is significant for promoting the development of application-level optoelectronic devices. To realize such devices, exploring the growth dynamics and interfacial carrier dynamics of perovskites deposited on the core materials of semiconductor technology is essential. Herein, we report the incommensurate heteroepitaxy of highly oriented single-crystal cesium lead bromide (CsPbBr3) on c-wurtzite GaN/sapphire substrates with atomically smooth surface and uniform rectangular shape by chemical vapor deposition. The CsPbBr3 microplatelet crystal exhibits green-colored lasing under room temperature and has a structural stability comparable with that grown on van der Waals mica substrates. Time-resolved photoluminescence spectroscopy studies show that the type-II CsPbBr3-GaN heterojunction effectively enhances the separation and extraction of free carriers inside CsPbBr3. These findings provide insights into the fabrication and application-level integrated optoelectronic devices of CsPbBr3 perovskites.

High-Quality Hexagonal Nonlayered CdS Nanoplatelets for Low-Threshold Whispering-Gallery-Mode Lasing.

Low threshold micro/nanolasers have attracted extensive attention for wide applications in high-density storage and optical communication. However, constrained by quantum efficiency and crystalline quality, conventional semiconductor small-sized lasers are still subjected to a high lasing threshold. In this work, a low-threshold planar laser based on high-quality single-crystalline hexagonal CdS nanoplatelets (NPLs) using a self-limited epitaxial growth method is demonstrated. The as-grown CdS NPLs show multiple whispering-gallery-mode lasing at room temperature with a threshold of ≈0.6 µJ cm-2 , which is the lowest value among reported CdS-based lasers. Through power-dependent lasing studies at 77 K, the lasing action is demonstrated to originate from a exciton-exciton scattering process. Furthermore, the edge length- and thickness-dependent lasing threshold studies reveal that the threshold is inversely proportional to the second power of lateral edge length while partially affected by vertical thickness, and the lasing modes can be sustained in NPLs as thin as 60 nm. The lowest threshold emerges with the thickness of ≈110 nm due to stronger energy confinement in the vertical Fabry-Pérot cavity. The results not only open up a new avenue to fabricate nonlayered material-based coherent light sources, but also advocate the promise of nonlayered semiconductor materials for the development of novel optoelectronic devices.

Charge-Transfer-Induced Photoluminescence Properties of WSe2 Monolayer-Bilayer Homojunction.

The charge-transfer process in transition-metal dichalcogenides (TMDCs) lateral homojunction affects the electron-hole recombination process of in optoelectronic devices. However, the optical properties of the homojunction reflecting the charge-transfer process has not been observed and studied. In this work, we investigated the charge-transfer-induced emission properties based on monolayer (1L)-bilayer (2L) WSe2 lateral homojunction with dozens of nanometer monolayer region. On the one hand, the photoluminescence (PL) emission of bilayer WSe2 from the homojunction area blue shifts ∼23 and ∼31 meV for direct and indirect bandgap emission, respectively, compared with the bare WSe2 bilayer region. The blue shift of the emission spectrum in the bilayer WSe2 is ascribed to the decrease in binding energy induced by charge transfer from monolayer to bilayer. On the other hand, the energy shift shows a tendency to increase as the temperature decreases. The energy blue shift is ∼57 meV for direct bandgap emission at 80 K, which is larger than that (∼23 meV) at room temperature. The larger-energy blue shift at low temperature is derived from the larger driving force under larger band offset. Our observations of the unique optical properties induced by efficient charge transfer are very helpful for exploring novel TMDC-based optoelectronic devices.

Low Threshold Fabry-Pérot Mode Lasing from Lead Iodide Trapezoidal Nanoplatelets.

Lead Iodide (PbI2 ) is a layered semiconductor with direct band gap holding great promises in green light emission and detection devices. Recently, PbI2 planar lasers are demonstrated using hexagonal whispering-gallery-mode microcavities, but the lasing threshold is quite high. In this work, lasing from vapor phase deposition derived PbI2 trapezoidal nanoplatelets (NPs) with threshold that is at least an order of magnitude lower than the previous value is reported. The growth mechanism of the trapezoidal NPs is explored and attributed to the synergistic effects of van der Waals interactions and lattice mismatching. The lasing is enabled by the population inversion of n = 1 excitons and the optical feedback is provided by the Fabry-Pérot oscillation between the side facets of trapezoidal NPs. The findings not only advance the understanding of growth and photophysics mechanism of PbI2 nanostructures but also provide ideas to develop low threshold ultrathin lasers.

Ultrathin CsPbX3 Nanowire Arrays with Strong Emission Anisotropy.

1D nanowires of all-inorganic lead halide perovskites represent a good architecture for the development of polarization-sensitive optoelectronic devices due to their high absorption efficient, emission yield, and dielectric constants. However, among as-fabricated perovskite nanowires with the lateral dimensions of hundreds nanometers so far, the optical anisotropy is hindered and rarely explored owing to the invalidating of electrostatic dielectric mismatch in the physical dimensions. Here, well-aligned CsPbBr3 and CsPbCl3 nanowires with thickness T down to 15 and 7 nm, respectively, are synthesized using a vapor phase van der Waals epitaxial method. Strong emission anisotropy with polarization ratio up to ≈0.78 is demonstrated in the nanowires with T < 40 nm due to the electrostatic dielectric confinement. With the increasing of thickness, the polarization ratio remarkably reduces monotonously to ≈0.17 until T ≈140 nm; and further oscillates in a small amplitude owing to the wave characteristic of light. These findings not only represent a demonstration of perovskite-based polarization-sensitive light sources, but also advance fundamental understanding of their polarization properties of perovskite nanowires.

Unveiling Structurally Engineered Carrier Dynamics in Hybrid Quasi-Two-Dimensional Perovskite Thin Films toward Controllable Emission.

Quasi-two-dimensional Ruddlesden-Popper perovskites driving carrier self-separation have rapidly advanced the development of high-performance optoelectronic devices. However, insightful understanding of carrier dynamics in the perovskites is still inadequate. The distribution of multiple perovskite phases, crucial for carrier separation, is controversial. Here we report a systematic study on carrier dynamics of spin-coated (C6H5CH2CH2NH3)2(CH3NH3)n-1PbnI3n+1 (n = 3 and 5) perovskite thin films. Efficient electrons transfer from small-n to large-n perovskite phases, and holes transfer reversely with time scales from ∼0.3 to 30.0 ps. The multiple perovskite phases are arranged perpendicularly to substrate from small to large n and also coexist randomly in the same horizontal planes. Further, the carrier separation dynamics is tailored by engineering the crystalline structure of the perovskite film, which leads to controllable emission properties. These results have important significance for the design of optoelectronic devices from solar cells, light-emitting diodes, lasers, and so forth.