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.

Micrometer-Resolution X-ray Imaging Enabled by a Flexible Perovskite Screen.

Spatial resolution improvement has been keenly sought recently in the perovskite-based scintillation community. Here, micrometer resolution (∼2.0 µm) was achieved by using an X-ray imaging screen of self-assembled perovskite nanosheets. The assembly behavior of nanosheets was applicable to many substrates, including glass, metal, and polymer surfaces. The use of a polymer substrate not only eliminated the parasite absorption of X-ray but also enabled a flexible screen with robust bending stability. The assembly behavior, on the other hand, provided vicinity for an efficient energy transfer between nanosheets of varied thicknesses, as evidenced by both transient absorption and photoluminescence lifetime measurements. Importantly, the ensuing large Stokes shift (∼316 meV) significantly mitigated the reabsorption issue, leading to a comparable light yield to LYSO/Ce crystals. With the aid of the synchrotron-based collimated X-ray beam, the fine structure of two-dimensional objects, such as microchips, was clearly visualized with the flexible scintillation screen. Furthermore, those challenging biological samples were also scanned by phase-contrast imaging, whereby a three-dimensional reconstruction was obtained successfully. Despite the labile nature of the perovskite screen, this work represents the state-of-the-art spatial resolution for perovskite scintillation.

Electrically Pumped Polarized Exciton-Polaritons in a Halide Perovskite Microcavity.

Recently, exciton-polaritons in lead halide perovskite microcavities have been extensively investigated to address striking phenomena such as polariton condensation and quantum emulation. However, a critical step in advancing these findings into practical applications, i.e., realizing electrically pumped perovskite polariton light-emitting devices, has not yet been presented. Here, we devise a new method to combine the device with a microcavity and report the first halide perovskite polariton light-emitting device. Specifically, the device is based on a CsPbBr3 capacitive structure, which can inject the electrons and holes from the same electrode, conducive to the formation of excitons and simultaneously maintaining the high quality of the microcavity. In addition, highly polarized polariton emissions have been demonstrated due to the optical birefringence in the CsPbBr3 microplate. This work paves the way for realizing practical polaritonic devices such as high-speed light-emitting devices for information communications and inversionless electrically pumped lasers based on perovskites.

Understanding Electron-Phonon Interactions in 3D Lead Halide Perovskites from the Stereochemical Expression of 6s2 Lone Pairs.

The electron-phonon (e-ph) interaction in lead halide perovskites (LHPs) plays a role in a variety of physical phenomena. Unveiling how the local lattice distortion responds to charge carriers is a critical step toward understanding the e-ph interaction in LHPs. Herein, we advance a fundamental understanding of the e-ph interaction in LHPs from the perspective of stereochemical activity of 6s2 lone-pair electrons on the Pb2+ cation. We demonstrate a model system based on three LHPs with distinctive lone-pair activities for studying the structure-property relationships. By tuning the A-cation chemistry, we synthesized single-crystal CsPbBr3, (MA0.13EA0.87)PbBr3 (MA+ = methylammonium; EA+ = ethylammonium), and (MHy)PbBr3 (MHy+ = methylhydrazinium), which exhibit stereo-inactive, dynamic stereo-active, and static stereo-active lone pairs, respectively. This gives rise to distinctive local lattice distortions and low-frequency vibrational modes. We find that the e-ph interaction leads to a blue shift of the band gap as temperature increases in the structure with the dynamic stereo-active lone pair but to a red shift in the structure with the static stereo-active lone pair. Furthermore, analyses of the temperature-dependent low-energy photoluminescence tails reveal that the strength of the e-ph interaction increases with increasing lone-pair activity, leading to a transition from a large polaron to a small polaron, which has significant influence on the emission spectra and charge carrier dynamics. Our results highlight the role of the lone-pair activity in controlling the band gap, phonon, and polaronic effect in LHPs and provide guidelines for optimizing the optoelectronic properties, especially for tin-based and germanium-based halide perovskites, where stereo-active lone pairs are more prominent than their lead counterparts.