Nonequilibrium transport in epitaxial CsPbBr3 single crystals

Abstract

Transport of optically excited carriers in semiconductors is typically described within a quasi-equilibrium picture, where energy is carried by a single thermalized quasiparticle population characterized by well-defined transport coefficients. Here, we demonstrate that in epitaxial CsPbBr3 perovskite single crystals, this picture holds near room temperature - but breaks down dramatically at low temperature. Using transient microscopy, we show that optically measured carrier mobilities match device-scale Hall-effect and field-effect transistor measurements across a broad temperature range, resolving reported discrepancies and validating the equilibrium framework in the free-carrier regime. Below ~60 K, however, when excitonic effects become significant, equilibrium models begin to fail. We observe two coupled populations: a transient (<100 ps) hot-exciton gas with a diffusivity ~25-30 cm 2 /s - greatly exceeding the diffusivity expected for thermalized excitons - and a quasi-localized state that is fed by the cooling of the hot-exciton gas. These results reveal that in CsPbBr3, transport and thermalization are not separable processes: carriers move while still redistributing among internal degrees of freedom, breaking the timescale separation that underpins equilibrium transport theory in conventional semiconductors. By resolving transport at the population level, we can directly access the competing kinetics of exciton formation, interconversion, and cooling, offering a new space for controlling energy flow in perovskite materials and their photonic applications.