Coherent ultrafast dynamics in functional molecular materials mediated by vibronic couplings

The ultrafast dynamics of non-equilibrium excitations in functional materials and nanostructures, induced by light-matter interactions, arise from a complex interplay between electronic and vibrational motion. Vibronic couplings can significantly influence the initial energy flow and charge motion following photoexcitation. A deep understanding of the underlying physics of photoinduced ultrafast phenomena is crucial for controlling nanoscale energy and charge transport, for the rationale design of efficient new materials and development of quantum technologies. Most of the mechanisms underlying these processes occur on only few 100s-fs timescales, thus demanding methods combining high time resolution and the ability to unravel couplings. Here, I will present our latest findings demonstrating how two-dimensional electronic spectroscopy with sub-10-fs time resolution provides detailed, new insights into the ultrafast coherent dynamics of technologically relevant molecular materials, and the fundamental role of vibronic couplings in these dynamics.