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Dynamical processes in ultralong-range Rydberg molecules


Ultralong-range Rydberg molecules (ULRMs) represent a new kind of molecular species with a unique binding mechanism and extraordinary properties. The prototype of a diatomic ULRM is composed of a ground state atom bound to a Rydberg atom where the binding occurs due to the scattering of the low-energy Rydberg electron from the polarizable ground state atom. ULRMs are of highly unbalanced character in the sense that typical Rydberg atoms with the principle quantum number ranging from ten to a few hundred vary in size from ten nanometers to a few micrometers whereas the ground state atom is of Angstrom size. For this very reason, they inherit both the exceptional properties of the Rydberg atom, such as a huge size and sensitivity to external fields, as well as the localization and structural properties of the ground state partner atom.

In the present project, we aim at establishing a solid theoretical description of the time-dependent molecular quantum dynamics and dynamical processes in this exotic species. Situated at the interface of Rydberg physics and quantum chemistry as well as quantum molecular dynamics, our work addresses in particular the interplay of ’coherent electronic and nuclear motion in Rydberg systems’ and the question of ’how to use electronic motion to initiate directed nuclear motion’.

We will perform wave-packet dynamical investigations and simulate the coherent motion of the nuclei in the molecular potential energy landscape for the dynamics in a single Born-Oppenheimer potential surface, but in particular also for quantum scattering involving several potential surfaces which are close in energy or even cross. Our simulations will range from the study of small and large amplitude oscillations to inelastic decays, charge transfer and atom ion-interactions. It will be the first study of the complete quantum dynamical evolution of one or more ground state atoms in the electronic cloud of a Rydberg atom. Our work will provide key input for the realization and interpretation of experiments probing the dynamics of ULRM such as pump-probe experiments.

Principal Investigator

Peter Schmelcher, Universitaet Hamburg

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