In Situ Exploration of the Structural Transition during Morphology- and Efficiency-Conserving Halide Exchange on a Single Perovskite Nanocrystal

摘要

Controlled fabrication of semiconductor nanostructures with unique physicochemical properties is vital for future technologies. In this study, transformation from red-emitting metal halide perovskite CH3NH3PbI3 nanocrystals (NCs) to green-emitting CH3NH3PbBr3 NCs was achieved without significant morphological changes and loss of photoluminescence (PL) efficiency via a controlled halide exchange reaction. In situ single-particle PL imaging along with detailed structural and elemental characterizations revealed that sudden cooperative transitions between two light-emitting states via intermediate dark states with >100 s durations during halide exchange originate from two distinct defect-mediated reconstruction processes with different activation energies (0.072 and 0.40 eV), leading to an isokinetic temperature of ca. 314 K, across a solid-state miscibility gap between the I- and Br-rich phases inside a single NC.