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arXiv · 2211.16344

Vibronic interactions in trilobite and butterfly Rydberg molecules

Frederic Hummel·Peter Schmelcher·Matthew T. Eiles
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Abstract

Ultralong-range Rydberg molecules provide an exciting testbed for molecular physics at exaggerated scales. In the so-called trilobite and butterfly Rydberg molecules, the Born-Oppenheimer approximation can fail due to strong non-adiabatic couplings arising from the combination of radial oscillations and rapid energy variations in the adiabatic potential energy curves. We utilize an accurate coupled-channel treatment of the vibronic system to observe the breakdown of Born-Oppenheimer physics, such as non-adiabatic trapping and decay of molecular states found near pronounced avoided crossings in the adiabatic potential curves. Even for vibrational states localized far away from avoided crossings, a single channel model is quantitatively sufficient only after including the diagonal non-adiabatic corrections to the Born-Oppenheimer potentials. Our results indicate the importance of including non-adiabatic physics in the description of ultralong-range Rydberg molecules and in the interpretation of measured vibronic spectra.

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Frederic Hummel, Peter Schmelcher, Matthew T. Eiles. 2022-11-29. Vibronic interactions in trilobite and butterfly Rydberg molecules. https://doi.org/10.1103/physrevresearch.5.013114

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