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The onset of collision dynamics between an ion and a Rydberg atom is studied in a regime characterized by a multitude of collision channels. These channels arise from coupling between a nonpolar Rydberg state and numerous highly polar Stark states. The interaction potentials formed by the polar Stark states show a substantial difference in spatial gradient compared to the nonpolar state leading to a separation of collisional timescales, which is observed in situ. For collision energies in the range of k_{B}μK to k_{B}K, the dynamics exhibit a counterintuitive dependence on temperature, resulting in faster collision dynamics for cold-initially "slow"-systems. Dipole selection rules enable us to prepare the collision pair on the nonpolar potential in a highly controlled manner, which determines occupation of the collision channels. The experimental observations are supported by semiclassical simulations, which model the pair state evolution and provide evidence for tunable nonadiabatic dynamics.

Vibrational dynamics in conventional molecules usually takes place on a timescale of picoseconds or shorter. A striking exception are ultralong-range Rydberg molecules, for which dynamics is dramatically slowed down as a consequence of the huge bond length of up to several micrometers. Here, we report on the direct observation of vibrational dynamics of a recently observed Rydberg-atom-ion molecule. By applying a weak external electric field of a few millivolts per centimeter, we are able to control the orientation of the photoassociated ultralong-range Rydberg molecules and induce vibrational dynamics by quenching the electric field. A high resolution ion microscope allows us to detect the molecule's orientation and its temporal vibrational dynamics in real space. Our study opens the door to the control of molecular dynamics in Rydberg molecules.

Atoms with a highly excited electron, called Rydberg atoms, can form unusual types of molecular bonds 1-4 . The bonds differ from the well-known ionic and covalent bonds 5,6 not only by their binding mechanisms, but also by their bond lengths ranging up to several micrometres. Here we observe a new type of molecular ion based on the interaction between the ionic charge and a flipping-induced dipole of a Rydberg atom with a bond length of several micrometres. We measure the vibrational spectrum and spatially resolve the bond length and the angular alignment of the molecule using a high-resolution ion microscope 7 . As a consequence of the large bond length, the molecular dynamics is extremely slow. These results pave the way for future studies of spatio-temporal effects in molecular dynamics (for example, beyond Born-Oppenheimer physics)., (© 2022. The Author(s), under exclusive licence to Springer Nature Limited.)