Coexistence of Incoherent and Ultrafast Coherent Exciton Transport in a Two-Dimensional Superatomic Semiconductor

Abstract

Fully leveraging the remarkable properties of low-dimensional semiconductors requires developing a deep understanding of how their structure and disorder affect the flow of electronic energy. Here, we study exciton transport in single crystals of the two-dimensional superatomic semiconductor CsRe₆Se₈I₃, which straddles a photophysically rich yet elusive intermediate electronic-coupling regime. Using femtosecond scattering microscopy to directly image exciton transport in CsRe₆Se₈I₃, we reveal the rare coexistence of coherent and incoherent exciton transport, leading to either persistent or transient electronic delocalization depending on temperature. Notably, coherent excitons exhibit ballistic transport at speeds approaching an extraordinary 1600 km/s over 300 fs. Such fast transport is mediated by J-aggregate-like superradiance, owing to the anisotropic structure and long-range order of CsRe₆Se₈I₃. Our results establish superatomic crystals as ideal platforms for studying the intermediate electronic-coupling regime in highly ordered environments, in this case displaying long-range electronic delocalization, ultrafast energy flow, and a tunable dual transport regime.