Abstract
Interfaces between molecules and 2D materials exhibit energy-driven functionalities, wherein charge transfer directs molecular motion. Unlike equilibrium systems, where molecular assemblies settle into static configurations, continuous energy input can drive transient, collective molecular rearrangements. Here, we reveal ultrafast spectroscopic fingerprints of a collective rotational response of molecules on a 2D material following photoexcitation. Our results suggest that photoinduced charge transfer reshapes the interfacial energy potential, giving rise to macroscopic, unidirectional molecular rotation and the formation of a homochiral molecular arrangement. Using a multiplexed ultrafast photoemission spectroscopy approach, we simultaneously track electronic states, atomic positions, and orbital wavefunctions with femtosecond and sub-Ångström resolution. Multimodal valence and core electron emission analysis disentangles the intertwined electronic-structural dynamics of the molecule and the 2D material, revealing the dynamic modulation of charge distribution and intermolecular forces that drive collective molecular motion. Our findings open a pathway for designing energy-driven molecular systems with tunable interfacial dynamics, with potential applications in chiral engineering and active matter systems.