Photodissociation of long-range Rydberg molecules

We present photodissociation of ultracold long-range Rydberg molecules as a tool to characterize their electronic properties. We photoassociate K-39(2) 37 P-2 molecules with highly entangled electronic and nuclear spins of the two bound atoms and quantify the entanglement by projection of the molecular state onto noninteracting atoms using radio-frequency photodissociation. By comparison of experimental photodissociation rates with theoretical predictions, we further characterize the electronic and nuclear wave function of the photoassociated molecules. Based on the complete characterization of the formed long-range Rydberg molecules, we demonstrate a full hyperfine-spin flip of a free ground-state atom through the interaction with a Rydberg atom.