Elucidation of Photoluminescence Blinking Mechanism and Multiexciton Dynamics in Hybrid Organic–Inorganic Perovskite Quantum Dots

Abstract Halide perovskites (ABX₃) have emerged as promising materials in the past decade owing to their superior photophysical properties, rendering them potential candidates as solar cells, light‐emitting diode displays, and lasing materials. To optimize their utilization into optoelectronic devices, fundamental understanding of the optical behaviors is necessary. To reveal the comprehensive structure–property relationship, CH₃NH₃PbBr₃ (MAPbBr₃) perovskite quantum dots (PQDs) of three different sizes are prepared by controlling the precipitation temperature. Photoluminescence (PL) blinking, a key process that governs the emission efficiency of the PQD materials, is investigated in detail by the time‐resolved spectroscopic measurements of individual dots. The nature of the generated species in the course of blinking events is identified, and the mechanism governing the PL blinking is studied as a function of PQD sizes. Further, the practical applicability of MAPbBr₃ PQDs is assessed by studying the multiexciton dynamics under high photoexcitation intensity under which most of the display devices work. Ultrafast transient absorption spectroscopy helped in uncovering the volume‐dependent Auger recombination rates, which are further explored by comparing the early‐time transitions related to surface trap states and higher band states.