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Vibronic quantum dynamics of ultralong-range high-ℓ Rydberg molecules

Felix Giering, Rohan Srikumar, and Peter Schmelcher

  • Zentrum für Optische Quantentechnologien, Universität Hamburg, Luruper Chaussee 149, 22761 Hamburg, Germany

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Phys. Rev. A 114, 022813 – Published 13 August, 2026

DOI: https://doi.org/10.1103/j7qc-6fww

Abstract

We investigate the nonadiabatic quantum dynamics of ultralong-range Rydberg molecules using a vibronically coupled two-channel treatment. The two channels are composed of coupled trilobite and butterfly electronic states, formed as a result of S-wave and P-wave scattering of high angular momentum Rydberg electrons with perturbing ground state atoms. Within the Born-Oppenheimer treatment, the P-wave scattering channel introduces an adiabatic decay pathway that affects the stability and lifetimes of trilobite states. Our numerical results show that the vibronic coupling is dependent on the principal quantum number n, and for certain n there is nonadiabatic stabilization against internal molecular decay, facilitating previously studied dynamical effects in pure trilobite molecules. Apart from the internal diffraction effect caused by the backscattering of vibrational wavepackets from the trilobite potential, we also observe interesting multiwell tunneling effects during low-energy oscillations for a range of n values. Our work serves to highlight the fact that the unique vibrational coordinate dependent electronic structure of these polar molecules, along with high-level densities, promises many exciting dynamical effects.

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Phys. Rev. A 114, 022813– Published 13 August, 2026
  • Received 17 March 2026
  • Accepted 16 July 2026
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