Vibrationally highly excited trilobite molecules stabilized by non-adiabatic coupling

Abstract: We report on the observation of highly excited ($\nu \sim 100)$ vibrational states of a trilobite ultralong-range Rydberg molecule in $<sup>{87}$Rb. These states manifest spectroscopically in a regularly spaced series of peaks red-detuned from the $25f_{7/2}$ dissociation threshold. The existence and observed stability of these states requires 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 wavepackets formed from high-lying vibrational states.