Coherent real-time charge transport across a donor−acceptor interface

We theoretically have studied the ultrafast charge transport in thiophene:fullerene stacks using time-dependent density functional tight-binding theory combined with Ehrenfest molecular dynamics for open systems. Our results reveal coherent oscillations of the charge density between neighboring donor sites, persisting for ∼200 fs and promoting charge transport within the polymer stacks. At the donor−acceptor interface, vibronic wave packets are launched, propagating coherently over distances of more than 3 nm into the acceptor region. This supports previous experimental observations of long-range ballistic charge-carrier motion in organic photovoltaic systems and highlights the importance of vibronic coupling engineering as a concept for tailoring the functionality of hybrid organic devices.