Unveiling high-mobility hot carriers in a two-dimensional conjugated coordination polymer

Abstract Hot carriers, inheriting excess kinetic energy from high-energy photons, drive numerous optoelectronic applications reliant on non-equilibrium transport processes. Although extensively studied in inorganic materials, their potential in organic-based systems remains largely unexplored. Here we demonstrate highly mobile hot carriers in crystalline two-dimensional conjugated coordination polymer Cu 3 BHT (BHT, benzenehexathiol) films. Leveraging a suite of ultrafast spectroscopic and imaging techniques, we map the microscopic charge transport landscape in Cu 3 BHT films following non-equilibrium photoexcitation across temporal, spatial and frequency domains, revealing two distinct high-mobility transport regimes. In the non-equilibrium regime, hot carriers achieve an ultrahigh mobility of ~2,000 cm 2 V –1 s –1 , traversing grain boundaries up to ~300 nm within a picosecond. In the quasi-equilibrium regime, free carriers exhibit Drude-type, band-like transport with a remarkable mobility of ~400 cm 2 V –1 s –1 and an intrinsic diffusion length exceeding 1 μm. These findings position two-dimensional conjugated coordination polymers as versatile platforms for advancing organic-based hot carrier applications.