Visualizing Three-Dimensional Quantum Fluctuations of Ground-State C${}_3$H${}_4$ via Deep Sub-Angstrom Coulomb Explosion Imaging

Coulomb explosion imaging (CEI) is a powerful tool for determining static geometries of isolated gas-phase molecules. In this work, taking allene and propyne as prototype, we demonstrate sub-angstrom resolution achieved with highly charged ion-induced CEI. Using 41.9 keV/u Xe${}^{20+}$ beam, minute variations of CC single, double and triple bond lengths are clearly visualized, indicating that an ultrahigh resolution of 0.1 $\mathring{\mathrm{A}}$ is achieved. This unprecedented resolution not only makes it possible to distinguish CC bonds with different bond orders, but also lays a solid foundation for direct observation of quantum fluctuations inherent to 3D structure of a ground-state molecule. Notably, the coupled collective motion of the two CH${}_2$ moieties spaced by a central carbon within allene is unambiguously visualized in our measurements.