Photophysical Properties of Submicrometer Ultrathin Perovskite Single-Crystal Films.

Organic-inorganic hybrid perovskite (OIHP) has attracted a great deal of interest with respect to diverse optoelectronic devices. However, the photophysical properties of the OIHP require further understanding because most of the investigations have been conducted with polycrystalline perovskites, which contain high-density structural defects. Here, diverse photophysical properties, including structural characterization, spectroscopic features, and photoexcited products, are studied in submicrometer CH3NH3PbBr3 ultrathin single-crystal (UTSC) films. Unlike polycrystalline films and large single crystals, the UTSC film provides a unique platform for studying spectroscopic characteristics of single-crystal perovskites. Compared with the polycrystalline film, the UTSC film presents an atomically flat morphology and near-perfect lattice with a lower defect density, leading to an isotropic system that can be applied in the construction of high-performance optoelectronic devices. Furthermore, a long lifetime emissive channel assigned to the trion is indicated, which is scarcely found in perovskite polycrystalline films. Our results profoundly improve our understanding of their photophysical properties and expand the horizons for perovskite materials in photonic applications.

Direct Hot-Electron Transfer at the Au Nanoparticle/Monolayer Transition-Metal Dichalcogenide Interface Observed with Ultrahigh Spatiotemporal Resolution.

Plasmon-induced hot-electron transfer at the metallic nanoparticle/semiconductor interface is the basis of plasmon-enhanced photocatalysis and energy harvesting. However, limited by the nanoscale size of hot spots and femtosecond time scale of hot-electron transfer, direct observation is still challenging. Herein, by using spatiotemporal-resolved photoemission electron microscopy with a two-color pump-probe beamline, we directly observed such a process with a concise system, the Au nanoparticle/monolayer transition-metal dichalcogenide (TMD) interface. The ultrafast hot-electron transfer from Au nanoparticles to monolayer TMDs and the plasmon-enhanced transfer process were directly measured and verified through an in situ comparison with the Au film/TMD interface and free TMDs. The lifetime at the Au nanoparticle/MoSe2 interface decreased from 410 to 42 fs, while the photoemission intensities exhibited a 27-fold increase compared to free MoSe2. We also measured the evolution of hot electrons in the energy distributions, indicating the hot-electron injection and decay happened in an ultrafast time scale of ∼50 fs without observable electron cooling.

Bright and Dark Quadrupolar Excitons in the WSe_{2}/MoSe_{2}/WSe_{2} Heterotrilayer.

Transition metal dichalcogenide heterostructures have been extensively studied as a platform for investigating exciton physics. While heterobilayers such as WSe_{2}/MoSe_{2} have received significant attention, there has been comparatively less research on heterotrilayers, which may offer new excitonic species and phases, as well as unique physical properties. In this Letter, we present theoretical and experimental investigations on the emission properties of quadrupolar excitons (QXs), a newly predicted type of exciton, in a WSe_{2}/MoSe_{2}/WSe_{2} heterotrilayer device. Our findings reveal that the optical brightness or darkness of QXs is determined by horizontal mirror symmetry and valley and spin selection rules. Additionally, the emission intensity and energy of both bright and dark QXs can be adjusted by applying an out-of-plane electric field, due to changes in hole distribution and the Stark effect. These results not only provide experimental evidence for the existence of QXs in heterotrilayers but also uncover their novel properties, which have the potential to drive the development of new exciton-based applications.

Highly Efficient Light-Emitting Diodes Based on Self-Assembled Colloidal Quantum Wells.

Nanocrystal-based light-emitting diodes (Nc-LEDs) have immense potential for next-generation high-definition displays and lighting applications. They offer numerous advantages, such as low cost, high luminous efficiency, narrow emission, and long lifetime. However, the external quantum efficiency (EQE) of Nc-LEDs, typically employing isotropic nanocrystals, is limited by the out-coupling factor. Here efficient, bright, and long lifetime red Nc-LEDs based on anisotropic nanocrystals of colloidal quantum wells (CQWs) are demonstrated. Through modification of the substrate's surface properties and control of the interactions among CQWs, a self-assembled layer with an exceptionally high distribution of in-plane transitions dipole moment of 95%, resulting in an out-coupling factor of 37% is successfully spin-coated. The devices exhibit a remarkable peak EQE of 26.9%, accompanied by a maximum brightness of 55 754 cd m-2 and a long operational lifetime (T95 @100 cd m-2 ) over 15 000 h. These achievements represent a significant advancement compared to previous studies on Nc-LEDs incorporating anisotropic nanocrystals. The work is expected to provide a general self-assembly strategy for enhancing the light extraction efficiency of Nc-LEDs based on anisotropic nanocrystals.