Exploring the vibrational series of pure trilobite Rydberg molecules.

In trilobite Rydberg molecules, an atom in the ground state is bound by electron-atom scattering to a Rydberg electron that is in a superposition of high angular momentum states. This results in a homonuclear molecule with a permanent electric dipole moment in the kilo-debye range. Trilobite molecules have previously been observed only with admixtures of low-l states. Here we report on the observation of two vibrational series of pure trilobite Rubidium-Rydberg molecules that are nearly equidistant. They are produced by three-photon photoassociation and lie energetically more than 15 GHz below the atomic 22F state of rubidium. We show that these states can be used to measure the electron-atom scattering length at low energies in order to benchmark current theoretical calculations. In addition to measuring their kilo-Debye dipole moments, we also show that the molecular lifetime is increased compared to the 22F state due to the high-l character. The observation of an equidistant series of vibrational states opens the way to observe coherent molecular wave packet dynamics.

Diffusive-like redistribution in state-changing collisions between Rydberg atoms and ground state atoms.

Exploring the dynamics of inelastic and reactive collisions on the quantum level is a fundamental goal in quantum chemistry. Such collisions are of particular importance in connection with Rydberg atoms in dense environments since they may considerably influence both the lifetime and the quantum state of the scattered Rydberg atoms. Here, we report on the study of state-changing collisions between Rydberg atoms and ground state atoms. We employ high-resolution momentum spectroscopy to identify the final states. In contrast to previous studies, we find that the outcome of such collisions is not limited to a single hydrogenic manifold. We observe a redistribution of population over a wide range of final states. We also find that even the decay to states with the same angular momentum quantum number as the initial state, but different principal quantum number is possible. We model the underlying physical process in the framework of a short-lived Rydberg quasi-molecular complex, where a charge exchange process gives rise to an oscillating electric field that causes transitions within the Rydberg manifold. The distribution of final states shows a diffusive-like behavior.