  Function is dynamic and originates at atomic interfaces. Combining the
degrees of freedom of molecules with the peculiar properties of 2D quantum
materials can create novel functionality. Here, we report the manipulation and
ultrafast imaging of a unidirectional gearing motion in molecules on a 2D
quantum material. To visualize and disentangle the intertwined structural and
electronic dynamics of such a hybrid interface, we record a 'full molecular
movie' by imaging the atomic positions, the evolution of the molecular orbital
wavefunctions and the modification of electronic states of the substrate. In a
multimodal investigation in a single setup, we disentangle dynamics in valence
and core electrons of both the molecule and the surface with femtosecond and
sub-{\aa}ngstr\"om precision. The ultrafast rotational motion is fueled by the
transfer of hot holes into the molecules that results in 'supercharging' of the
film. As hot carriers move through the interface, we track a transient
modification of the frontier molecular orbitals and observe a chiral symmetry
breaking associated with local structural rearrangements. Our calculations show
that the 'supercharging' changes the interfacial potential energy landscape and
triggers the gearing motion. The experiment offers all-in-one imaging of the
electronic, molecular orbital, chemical and structural dynamics during the flow
of charge and energy across the hybrid interface. Our approach provides
detailed dynamical information on the mechanism underlying surface-adsorbed
molecular gears and enables tailoring novel functionalities in hybrid active
matter.
