Orbital-resolved imaging of coherent femtosecond exciton dynamics in coupled molecules

Optical excitation and control of excitonic wavepackets in organic molecules is the basis to energy conversion processes. To gain insights into such processes, it is essential to establish the relationship between the coherence timescales of excitons with the local electronic distribution in the molecules, as well as the influence of intermolecular interactions on exciton dynamics. Here, we demonstrate orbital-resolved imaging of optically induced coherent exciton dynamics in single copper naphthalocyanine (CuNc) molecules, and selective coherent excitation of dark and bright triplet excitons in coupled molecular dimers. Ultrafast photon-induced tunneling current enabled atomic-scale imaging and control of the excitons in resonantly excited molecules by employing excitonic wavepacket interferometry. Our results reveal an ultrafast exciton coherence time of ~ 70 fs in a single molecule, which decreases for the triplet excitons in interacting molecules.