Direct observation of geometric phase in dynamics around a conical intersection

Conical intersections are ubiquitous in chemistry, often governing processes such as light harvesting, vision, photocatalysis, and chemical reactivity. They act as funnels between electronic states of molecules, allowing rapid and efficient relaxation during chemical dynamics. In addition, when a reaction path encircles a conical intersection, the molecular wavefunction experiences a geometric phase, which affects the outcome of the reaction through quantum-mechanical interference. Past experiments have measured indirect signatures of geometric phases in scattering patterns and spectroscopic observables, but there has been no direct observation of the underlying wavepacket interference. Here, we experimentally observe geometric-phase interference in the dynamics of a nuclear wavepacket travelling around an engineered conical intersection in a programmable trapped-ion quantum simulator. To achieve this, we develop a new technique to reconstruct the two-dimensional wavepacket densities of a trapped ion. Experiments agree with the theoretical model, demonstrating the ability of analog quantum simulators—such as those realised using trapped ions—to accurately describe nuclear quantum effects. These results demonstrate a path to deploying analog quantum simulators for solving some of the most difficult problems in chemical dynamics.

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