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This study advances the theoretical understanding of ultralong-range Rydberg molecules by modeling non-adiabatic quantum dynamics in coupled trilobite and butterfly electronic states. The research identifies specific principal quantum numbers where vibronic coupling stabilizes these fragile systems against internal decay, revealing novel multi-well tunneling effects relevant to precision control of exotic matter. These findings deepen the fundamental knowledge base required for future applications involving Rydberg atom arrays and complex molecular simulations in quantum platforms.
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Vibronic quantum dynamics of ultralong-range high-$\ell$ Rydberg molecules

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arXiv:2603.15489v2 Announce Type: replace-cross Abstract: We investigate the non-adiabatic 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 non-adiabatic 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 multi-well tunneling effects during low-energy oscillations for a range of $n$-values. Our work serves to highlight that the unique vibrational coordinate dependent electronic structure of these polar molecules, along with high level densities, promise many exciting dynamical effects.

Abstract:We investigate the non-adiabatic 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 non-adiabatic 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 multi-well tunneling effects during low-energy oscillations for a range of $n$-values. Our work serves to highlight that the unique vibrational coordinate dependent electronic structure of these polar molecules, along with high level densities, promise many exciting dynamical effects.

Atomic Physics (physics.atom-ph); Quantum Physics (quant-ph)

arXiv:2603.15489 [physics.atom-ph]

(or arXiv:2603.15489v2 [physics.atom-ph] for this version)

https://doi.org/10.48550/arXiv.2603.15489 Focus to learn more arXiv-issued DOI via DataCite

Phys. Rev. A 114, 022813, 2026

https://doi.org/10.1103/j7qc-6fww Focus to learn more DOI(s) linking to related resources

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