All-inorganic cesium lead halide perovskite (CsPbX3, X = Cl, Br, and I) nanocrystals (NCs) are emerging as an important class of semiconductor materials with superior photophysical properties and wide potential applications in optoelectronic devices. So far, only a few studies have been conducted to control the shape and geometry of CsPbX3 NCs. Here we report a general approach to directly synthesize two-dimensional (2D) CsPbX3 perovskite and mixed perovskite nanosheets with uniform and ultrathin thicknesses down to a few monolayers. The key to the high-yield synthesis of perovskite nanosheets is the development of a new Cs-oleate precursor. The as-synthesized CsPbX3 nanosheets exhibit bright photoluminescence with broad wavelength tunability by composition modulation. The excellent optoelectronic properties of CsPbX3 nanosheets combined with their unique 2D geometry and large lateral dimensions make them ideal building blocks for building functional devices. To demonstrate their potential applications in optoelectronics, photodetectors based on CsPbBr3 nanosheets are fabricated, which exhibit high on/off ratios with a fast response time.
Discretely sized semiconductor clusters have attracted considerable attention due to their intriguing optical properties and self-assembly behaviors. While lead halide perovskite nanostructures have been recently intensively explored, few studies have addressed perovskite clusters and their self-assembled superstructures. Here, we report the room-temperature synthesis of sub-2 nm CsPbBr clusters and present strong evidence that these ultrasmall perovskite species, obtained under a wide range of reaction conditions, possess a specific size, with optical properties and self-assembly characteristics resembling those of well-known II-VI semiconductor magic-sized clusters. Unlike conventional CsPbBr nanocrystals, the as-synthesized CsPbBr nanoclusters spontaneously self-assemble into a hexagonally packed columnar mesophase in solution, which can be further converted to single-crystalline CsPbBr quantum nanoribbons with bright deep-blue emission at room temperature. Such a conversion of CsPbBr nanoclusters to nanoribbons is found to be driven by a ligand-destabilization-induced crystallization and mesophase transition process. Our study will facilitate the investigation of perovskite nanoclusters and offer new possibilities in the low-temperature synthesis of anisotropic perovskite nanostructures.
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