Kiana Baumgärtner, Misa Nozaki, Marvin Reuner, Nils Wind, Masato Haniuda, Christian Metzger, Michael Heber, Dmytro Kutnyakhov, Federico Pressacco, Lukas Wenthaus, Keisuke Hara, Kalyani Chordiya, Chul-Hee Min, Martin Beye, F. Reinert, Friedrich Roth, Sanjoy Kr Mahatha, Anders Madsen, Tim O. Wehling, Kaori Niki, Daria Popova-Gorelova, Kai Roßnagel, Markus Scholz
Abstract Interfaces between molecules and 2D material interfaces exhibit energy-driven functionalities (1–3 ), where charge transfer directs molecular motion (4–6) . Unlike equilibrium systems, where molecular assemblies settle into static configurations, continuous energy input can drive transient, collective molecular rearrangements. Here, we uncover the synchronized rotational motion of molecules on a 2D material following photoexcitation. We demonstrate that charge transfer reshapes the interfacial energy potential, inducing macroscopic, unidirectional molecular rotation and the formation of homochiral domains. Using a multiplexed ultrafast photoemission spectroscopy approach, we simultaneously track, electronic states (7–12) , atomic positions (13,14) and orbital wavefunctions (15,16) with femtosecond and sub-Ångström resolution. Multimodal valence and core electron emission analysis (17) 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.