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Observation of dipole-quadrupole interaction in an ultracold gas of Rydberg atoms

We observe the direct excitation of pairs of Cs atoms from the ground state to molecular states correlating asymptotically to $ns\,n'f$ asymptotes. The molecular resonances are interpreted as originating from the dipole-quadrupole interaction between the $ns\,n'f$ pair states and close-by $np\,np$ asymptotes ($22\leq n \leq 32$). This interpretation is supported by Stark spectroscopy of the pair states and a detailed modeling of the interaction potentials. The dipole-quadrupole interaction mixes electronic states of opposite parity and thus requires a coupling between electronic and nuclear motion to conserve the total parity of the system. This non-Born-Oppenheimer coupling is facilitated by the near-degeneracy of even and odd $L$ partial waves in the atom-atom scattering which have opposite parity.