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Ultralong-range Rydberg molecules (ULRM) are highly imbalanced bound systemsformed via the low-energy scattering of a Rydberg electron with a ground-stateatom. We investigate for $^{23}$Na the $d$-state and the energetically close-bytrilobite state, exhibiting avoided crossings that lead to the breakdown of theadiabatic Born-Oppenheimer (BO) approximation. We develop a coupled-channelapproach to explore the non-adiabatic interaction effects between theseelectronic states. The resulting spectrum exhibits stark differences incomparison to the BO spectra, such as the existence of above-threshold resonantstates without any adiabatic counterparts, and a significant rearrangement ofthe spectral structure as well as the localization of the eigenstates. Ourstudy motivates the use of $^{23}$Na ULRM, as a probe to explore vibronicinteraction effects on exaggerated time and length scales.

Non-adiabatic interaction effects in the spectra of ultralong-range Rydberg molecules