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Observation of geometric phase effect through backward angular oscillations in the H + HD → H2 + D reaction
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Observation of geometric phase effect through backward angular oscillations in the H + HD → H2 + D reaction
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Journal Article
Observation of geometric phase effect through backward angular oscillations in the H + HD → H2 + D reaction
2024
Overview
Quantum interference between reaction pathways around a conical intersection (CI) is an ultrasensitive probe of detailed chemical reaction dynamics. Yet, for the hydrogen exchange reaction, the difference between contributions of the two reaction pathways increases substantially as the energy decreases, making the experimental observation of interference features at low energy exceedingly challenging. We report in this paper a combined experimental and theoretical study on the H + HD → H
2
+ D reaction at the collision energy of 1.72 eV. Although the roaming insertion pathway constitutes only a small fraction (0.088%) of the overall contribution, angular oscillatory patterns arising from the interference of reaction pathways were clearly observed in the backward scattering direction, providing direct evidence of the geometric phase effect at an energy of 0.81 eV below the CI. Furthermore, theoretical analysis reveals that the backward interference patterns are mainly contributed by two distinct groups of partial waves (
J
~ 10 and
J
~ 19). The well-separated partial waves and the geometric phase collectively influence the quantum reaction dynamics.
In a combined experimental and theoretical study of the H + HD → H
2
+ D reaction at low collision energy (1.72 eV), the authors obtain detailed information on the quantum reaction dynamics surrounding a conical intersection.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
