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Vibrationally highly excited trilobite molecules stabilized by nonadiabatic coupling

Rohan Srikumar1,*, Markus Exner2,*, Richard Blättner2, Peter Schmelcher1,3, Matthew T. Eiles4, and Herwig Ott2,†

  • *These authors contributed equally to this work.
  • †Contact author: ott@physik.uni-kl.de

Phys. Rev. Research 7, 043103 – Published 27 October, 2025

DOI: https://doi.org/10.1103/49ky-d8mm

Abstract

We report on the observation of highly excited (ν∼100) vibrational states of a trilobite ultralong-range Rydberg molecule in Rb87. These states manifest spectroscopically in a regularly spaced series of peaks red-detuned from the 25f7/2 dissociation threshold. The existence and observed stability of these states require the almost complete suppression of the adiabatic decay pathway induced by the P-wave shape resonance of Rb. This stabilization is predicted to occur only for certain Rydberg levels where the avoided crossing between trilobite and P-wave-dominated butterfly potential energy curves nearly vanishes, allowing the vibrational states to diabatically traverse the crossing with almost unit probability. This is the first direct measurement of beyond-Born-Oppenheimer physics in long-range Rydberg molecules, and paves the way for future experiments to access and manipulate wave packets formed from high-lying vibrational states.

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