Intrinsic exciton transport and recombination in single-crystal lead bromide perovskite

Abstract

Photogenerated carrier transport and recombination in metal halide perovskites are critical to device performance. Despite considerable efforts, sample quality issues and measurement techniques have limited the access to their intrinsic physics. Here, by utilizing high-purity CsPbBr3 single crystals and contact-free transient grating spectroscopy, we directly monitor exciton diffusive transport from 26 to 300 K. As the temperature (T) increases, the carrier mobility ({\mu}) decreases rapidly below 100 K wtih a {\mu}~T^{-3.0} scaling, and then follows a more gradual {\mu}~T^{-1.7} trend at higher temperatures. First-principles calculations perfectly reproduce this experimental trend and reveal that optical phonon scattering governs carrier mobility shifts over the entire temperature range, with a single longitudinal optical mode dominating room-temperature transport. Time-resolved photoluminescence further identifies a substantial increase in exciton radiative lifetime with temperature, attributed to increased exciton population in momentum-dark states caused by phonon scattering. Our findings unambiguously resolve previous theory-experiment discrepancies, providing benchmarks for future optoelectronic design.