Direct Observation of Charge Collection at Nanometer-Scale Iodide-Rich Perovskites during Halide Exchange Reaction on CHNHPbBr.

Organolead halide perovskites MAPbX (MA = CHNH, X = Cl, Br, or I) are known to undergo reversible halide exchange reactions, enabling bandgap tuning over the visible light region. Using single-particle photoluminescence (PL) imaging for in situ observation, we have studied the structure-dependent charge dynamics during halide exchange with iodide ions on an MAPbBr crystal. In particular, we optically detected nanometer-scale iodide-rich domains (i.e., MAPbBrI) and found that their lifetimes of several tens of milliseconds are limited by reaction with diffusing vacancies. Furthermore, it was discovered that these domains effectively collect the charge carriers from the bulk crystal, thus resulting in amplified spontaneous emission (ASE) under continuous-wave laser irradiation. Our findings will provide direction for development of perovskite heterostructures with enhanced charge utilization.