Observation of the geometric phase effect in the H + HD → H₂ + D reaction

Daofu Yuan¹, Yafu Guan², Wentao Chen¹, Hailin Zhao², Shengrui Yu³, Chang Luo¹, Yuxin Tan¹, Ting Xie¹, Xingan Wang⁴, Zhigang Sun⁵, Dong H Zhang⁵, Xueming Yang^{5

6}

Affiliations

¹ Hefei National Laboratory for Physical Sciences at the Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei, 230026, China.
² State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
³ Hangzhou Institute of Advanced Studies, Zhejiang Normal University, Hangzhou, 311231, China.
⁴ Hefei National Laboratory for Physical Sciences at the Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei, 230026, China. xawang@ustc.edu.cn zsun@dicp.ac.cn zhangdh@dicp.ac.cn xmyang@dicp.ac.cn yangxm@sustc.edu.cn.
⁵ State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China. xawang@ustc.edu.cn zsun@dicp.ac.cn zhangdh@dicp.ac.cn xmyang@dicp.ac.cn yangxm@sustc.edu.cn.
⁶ Department of Chemistry, School of Science, Southern University of Science and Technology, Shenzhen, 518055, China.

PMID: 30545885
DOI: 10.1126/science.aav1356

Observation of the geometric phase effect in the H + HD → H₂ + D reaction

Daofu Yuan et al. Science. 2018.

. 2018 Dec 14;362(6420):1289-1293.

doi: 10.1126/science.aav1356.

Authors

Daofu Yuan¹, Yafu Guan², Wentao Chen¹, Hailin Zhao², Shengrui Yu³, Chang Luo¹, Yuxin Tan¹, Ting Xie¹, Xingan Wang⁴, Zhigang Sun⁵, Dong H Zhang⁵, Xueming Yang^{5

6}

Affiliations

¹ Hefei National Laboratory for Physical Sciences at the Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei, 230026, China.
² State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
³ Hangzhou Institute of Advanced Studies, Zhejiang Normal University, Hangzhou, 311231, China.
⁴ Hefei National Laboratory for Physical Sciences at the Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei, 230026, China. xawang@ustc.edu.cn zsun@dicp.ac.cn zhangdh@dicp.ac.cn xmyang@dicp.ac.cn yangxm@sustc.edu.cn.
⁵ State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China. xawang@ustc.edu.cn zsun@dicp.ac.cn zhangdh@dicp.ac.cn xmyang@dicp.ac.cn yangxm@sustc.edu.cn.
⁶ Department of Chemistry, School of Science, Southern University of Science and Technology, Shenzhen, 518055, China.

PMID: 30545885
DOI: 10.1126/science.aav1356

Abstract

Theory has established the importance of geometric phase (GP) effects in the adiabatic dynamics of molecular systems with a conical intersection connecting the ground- and excited-state potential energy surfaces, but direct observation of their manifestation in chemical reactions remains a major challenge. Here, we report a high-resolution crossed molecular beams study of the H + HD → H₂ + D reaction at a collision energy slightly above the conical intersection. Velocity map ion imaging revealed fast angular oscillations in product quantum state-resolved differential cross sections in the forward scattering direction for H₂ products at specific rovibrational levels. The experimental results agree with adiabatic quantum dynamical calculations only when the GP effect is included.

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Observation of the geometric phase effect in the H + HD → H₂ + D reaction

Affiliations

Observation of the geometric phase effect in the H + HD → H₂ + D reaction

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