Controllable CsxFA1-xPbI3 Single-Crystal Morphology via Rationally Regulating the Diffusion and Collision of Micelles toward High-Performance Photon Detectors

Cs(x)FA(1-x)PbI(3) single crystals are expected to provide more excitement in optoelectronic applications, including photodetector, laser, light-emitting diode, etc. Herein, we aim to gain an in-depth understanding of the growth mechanisms of perovskite single crystal with various morphologies in view of microscopic dynamics by the combination of component, structure, and solvent engineering. A sequence of Cs(x)FA(1-x)PbI(3) (0 <= x <= 0.14) perovskite single crystals with a dodecahedron morphology and tunable aspect ratio can be obtained by means of a solution-processed uniform-cooling approach. The optimized Cs(0.1)FA(0.9)PbI(3) single crystals prepared in gamma-butyrolactone mixed with dimethyl sulfoxide are theoretically and experimentally demonstrated to have superior performances, e.g., extremely higher long-term stability, lower trap density, and higher mobility. The broadband absorption, i.e., 300-910 nm, enables its application in near-infrared detection (880 nm), and the corresponding detector demonstrates higher responsivity at different light intensities and a fast photocurrent response (tau(1) = 11 mu s, tau(2) = 10 mu s). Equally important, we also explore the application of optimized Cs(0.1)FA(0.9)PbI(3) single crystals with a tunable aspect ratio in an X-ray detector and the extremely high sensitivity (2772.1 mu C Gy(air)(-1) cm(-2) under a bias of 150 V) demonstrates their good potential for radiation detection.