Observation of geometric phase effect through backward angular oscillations in the H + HD → H2 + D reaction

Shihao Li, Jiayu Huang, Zhibing Lu, Yiyang Shu, Wentao Chen, Daofu Yuan, Tao Wang, Bina Fu, Zhaojun Zhang (), Xingan Wang (), Dong H. Zhang () and Xueming Yang ()
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Shihao Li: University of Science and Technology of China
Jiayu Huang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Zhibing Lu: University of Science and Technology of China
Yiyang Shu: University of Science and Technology of China
Wentao Chen: University of Science and Technology of China
Daofu Yuan: University of Science and Technology of China
Tao Wang: College of Science, Southern University of Science and Technology
Bina Fu: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Zhaojun Zhang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Xingan Wang: University of Science and Technology of China
Dong H. Zhang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Xueming Yang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences

Nature Communications, 2024, vol. 15, issue 1, 1-7

Abstract: Abstract 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 → H2 + 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.

Date: 2024
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DOI: 10.1038/s41467-024-45843-6

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