A Universal Assembly Strategy of All-Inorganic Non-Layered Perovskite Single Crystals for High-Responsivity Photodetectors

Non-layered all-inorganic perovskite single crystals (AIPSCs) have ultralow trap density and exceptional optoelectronic properties, which can be used for developing high-performance perovskite optoelectronic devices with high efficiency and stability. However, there is a lack of comprehensive insight and universal principles to guide the preparation of high-quality AIPSCs. Herein, a universal liquid-air interfacial assembly strategy is proposed for synthesizing non-layered AIPSCs, in virtue of which a series of AIPSCs including whole structural dimensions from 0D to 3D are acquired. Specially, the CsPbI3 AIPSCs exhibit an ultrathin thickness of 40 nm, and the CsPbBr3 AIPSCs show ultra-narrow PL FWHM of 11 nm. Photodetectors (PDs) based on CsPbBr3 show excellent performance with responsivity up to 120 A W-1 and detectivity exceeding 2 x 10(13) Jones. Moreover, vertically integrated heterojunctions of mixed-dimensions are fabricated, and the 2D/3D heterostructure PDs further display enhanced self-powered characteristics. This work provides general synthetic guidance toward the synthesis of non-layered AIPSCs and promotes their application in AIPSCs-based optoelectronics.