Super-diffusive sub-picosecond extraction of hot carriers in black phosphorous

Abstract

Harvesting hot carriers before they lose energy to the lattice is a critical route toward surpassing the conventional thermodynamic limit in optical-to-electrical (O-E) conversion. However, photocurrent from such hot carriers has remained challenging to directly detect because they equilibrate on picosecond timescales, outpacing conventional electronic measurement. Here, by employing terahertz electronics with sub-picosecond temporal resolution, we directly monitor hot-carrier-driven O-E conversion in black phosphorus (BP). Photoexcitation near the metal contact under zero source-drain bias generates an ultrafast photocurrent with a decay time of ~400 fs, orders of magnitude faster than the typical sub-nanosecond energy relaxation in BP, demonstrating a measured 3 dB bandwidth of 260 GHz with an intrinsic limit of ~600 GHz. Notably, this photocurrent flows via energetic holes toward the contact electrode, regardless of the equilibrium carrier type, revealing a super-diffusive hot-carrier extraction mechanism. Furthermore, we show that the ultrafast hot-carrier contribution can coexist with the much slower cold-carrier contribution based on the photovoltaic effect, demonstrating that hot carriers can be harvested without discarding lower-energy carriers. These findings highlight the potential of sub-picosecond hot-carrier extraction to expand the O-E conversion bandwidth without sacrificing efficiency, bridging fundamental hot-carrier physics with ultrahigh-speed technological applications.