Direct observation of geometric-phase interference in dynamics around a conical intersection

Conical intersections are ubiquitous in chemistry and physics, 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...

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Veröffentlicht in:Nature chemistry 2023-11, Vol.15 (11), p.1503-1508
Hauptverfasser: Valahu, C. H., Olaya-Agudelo, V. C., MacDonell, R. J., Navickas, T., Rao, A. D., Millican, M. J., Pérez-Sánchez, J. B., Yuen-Zhou, J., Biercuk, M. J., Hempel, C., Tan, T. R., Kassal, I.
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Sprache:eng
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Zusammenfassung:Conical intersections are ubiquitous in chemistry and physics, 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 can affect 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 wavepacket travelling around an engineered conical intersection in a programmable trapped-ion quantum simulator. To achieve this, we develop a technique to reconstruct the two-dimensional wavepacket densities of a trapped ion. Experiments agree with the theoretical model, demonstrating the ability of analogue quantum simulators—such as those realized using trapped ions—to accurately describe nuclear quantum effects. Wavepacket dynamics around conical intersections are influenced by geometric phase, which can affect chemical reaction outcomes but has only been observed through indirect signatures. Now, by engineering a controllable conical intersection in a trapped-ion quantum simulator, the destructive wavepacket interference caused by a geometric phase has been observed.
ISSN:1755-4330
1755-4349
DOI:10.1038/s41557-023-01300-3