Disrupted Attosecond Charge Carrier Delocalization at a Hybrid Organic/Inorganic Semiconductor Interface

Despite significant interest in hybrid organic/inorganic semiconductor interfaces, little is known regarding the fate of charge carriers at metal oxide interfaces, particularly on ultrafast time scales. Using core-hole clock spectroscopy, we investigate the ultrafast charge carrier dynamics of conductive ZnO films at a hybrid interface with an organic semiconductor. The adsorption of C60 on the ZnO surface strongly suppresses the ultrafast carrier delocalization and increases the charge carrier residence time from 400 attoseconds to nearly 30 fs. Here, we show that a new hybridized interfacial density of states with substantial molecular character is formed, fundamentally altering the observed carrier dynamics. The remarkable change in the dynamics sheds light on the fate of carriers at hybrid organic/inorganic semiconductor interfaces relevant to organic optoelectronics and provides for the first time an atomistic picture of the electronically perturbed near-interface region of a metal oxide.