Probing electronic state-dependent conformational changes in a trapped Rydberg ion Wigner crystal

TL;DR

This paper demonstrates the first experimental observation of state-dependent conformational changes in a trapped Rydberg ion Wigner crystal, revealing how electronic excitations can induce structural transformations and hybridize vibrational and electronic states.

Contribution

It presents the first experimental evidence of electronic state-dependent structural changes in a Rydberg ion crystal, emulating molecular conformational dynamics.

Findings

Observation of a transition from linear to zigzag configuration upon Rydberg excitation

Detection of strong hybridisation between vibrational and electronic states

Spectroscopic signatures indicating state-dependent conformational changes

Abstract

State-dependent conformational changes play a central role in molecular dynamics, yet they are often difficult to observe or simulate due to their complexity and ultrafast nature. One alternative approach is to emulate such phenomena using quantum simulations with cold, trapped ions. In their electronic ground state, these ions form long-lived Wigner crystals. When excited to high-lying electronic Rydberg states, the ions experience a modified trapping potential, resulting in a strong coupling between their electronic and vibrational degrees of freedom. In an ion crystal, this vibronic coupling creates electronic state-dependent potential energy surfaces that can support distinct crystal structures -- closely resembling the conformational changes of molecules driven by electronic excitations. Here, we present the first experimental observation of this effect, by laser-coupling a single ion at the centre of a three-ion crystal to a Rydberg state. By tuning the system close to a structural phase transition, the excitation induces a state-dependent conformational change, transforming the Wigner crystal from a linear to a zigzag configuration. This structural change leads to a strong hybridisation between vibrational and electronic states, producing a clear spectroscopic signature in the Rydberg excitation. Our findings mark the first experimental step towards using Rydberg ions to create and study artificial molecular systems. change leads to a strong hybridisation between vibrational and electronic states, producing a clear spectroscopic signature in the Rydberg excitation. Our findings mark the first experimental step towards using Rydberg ions to create and study artificial molecular systems.