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Perovskite nanocrystals (NCs) have become leading candidates for solution-processed optoelectronics applications. While substantial work has been published on 3-D perovskite phases, the NC form of the zero-dimensional (0-D) phase of this promising class of materials remains elusive. Here we report the synthesis of a new class of colloidal semiconductor NCs based on Cs4PbBr6, the 0-D perovskite, enabled through the design of a novel low-temperature reverse microemulsion method with 85% reaction yield. These 0-D perovskite NCs exhibit high photoluminescence quantum yield (PLQY) in the colloidal form (PLQY: 65%), and, more importantly, in the form of thin film (PLQY: 54%). Notably, the latter is among the highest values reported so far for perovskite NCs in the solid form. Our work brings the 0-D phase of perovskite into the realm of colloidal NCs with appealingly high PLQY in the film form, which paves the way for their practical application in real devices.

Hybrid organic-inorganic perovskite crystals have recently become one of the most important classes of photoactive materials in the solar cell and optoelectronic communities. Albeit improvements have focused on state-of-the-art technology including various fabrication methods, device architectures, and surface passivation, progress is yet to be made in understanding the actual operational temperature on the electronic properties and the device performances. Therefore, the substantial effect of temperature on the optoelectronic properties, charge separation, charge recombination dynamics, and photoconversion efficiency are explored. The results clearly demonstrated a significant enhancement in the carrier mobility, photocurrent, charge carrier lifetime, and solar cell performance in the 60 ± 5 °C temperature range. In this temperature range, perovskite crystal exhibits a highly symmetrical relaxed cubic structure with well-aligned domains that are perpendicular to a principal axis, thereby remarkably improving the device operation. This finding provides a new key variable component and paves the way toward using perovskite crystals in highly efficient photovoltaic cells.

Perovskite nanocrystals (NCs) have become leading candidates for solution-processed optoelectronics applications. While substantial work has been published on 3-D perovskite phases, the NC form of the zero-dimensional (0-D) phase of this promising class of materials remains elusive. Here we report the synthesis of a new class of colloidal semiconductor NCs based on Cs