Observation of the geometric phase effect in the H+HD -> H-2+D reaction below the conical intersection

Yuan, Daofu1,2; Huang, Yin3; Chen, Wentao1,2; Zhao, Hailin3; Yu, Shengrui4; Luo, Chang1,2; Tan, Yuxin1,2; Wang, Siwen1,2; Wang, Xingan1,2; Sun, Zhigang3; Yang, Xueming3,5

2020-07-20

10.1038/s41467-020-17381-4

Nature Communications   影响因子和分区

2041-1723

It has long been known that there is a conical intersection (CI) between the ground and first excited electronic state in the H-3 system. Its associated geometric phase (GP) effect has been theoretically predicted to exist below the CI since a long time. However, the experimental evidence has not been established yet and its dynamical origin is waiting to be elucidated. Here we report a combined crossed molecular beam and quantum reactive scattering dynamics study of the H+HD -> H-2+D reaction at 2.28 eV, which is well below the CI. The GP effect is clearly identified by the observation of distinct oscillations in the differential cross section around the forward direction. Quantum dynamics theory reveals that the GP effect arises from the phase alteration of a small part of the wave function, which corresponds to an unusual roaming-like abstraction pathway, as revealed by quasi-classical trajectory calculations. The geometric phase effect associated with a conical intersection between the ground and first excited electronic state has been predicted in the H-3 system below the conical intersection energy. The authors, by a crossed molecular beam technique and quantum dynamic calculations, provide experimental evidence and insight into its origin.

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英语

NI论文

通讯

National Key R&D Program of China[2016YFF0200500] ; National Natural Science Foundation of China[21688102][21825303] ; Strategic Priority Research Program of Chinese Academy of Sciences[XDB17000000]

Science & Technology - Other Topics

Multidisciplinary Sciences

WOS:000553545000005

NATURE PUBLISHING GROUP

Web of Science

1.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China
2.Univ Sci & Technol China, Dept Chem Phys, Hefei 230026, Peoples R China
3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China
4.Zhejiang Normal Univ, Hangzhou Inst Adv Studies, Hangzhou 311231, Peoples R China
5.Southern Univ Sci & Technol, Coll Sci, Dept Chem, Shenzhen 518055, Peoples R China

Yuan, Daofu,Huang, Yin,Chen, Wentao,et al. Observation of the geometric phase effect in the H+HD -> H-2+D reaction below the conical intersection[J]. Nature Communications,2020,11(1).

Yuan, Daofu.,Huang, Yin.,Chen, Wentao.,Zhao, Hailin.,Yu, Shengrui.,...&Yang, Xueming.(2020).Observation of the geometric phase effect in the H+HD -> H-2+D reaction below the conical intersection.Nature Communications,11(1).

Yuan, Daofu,et al."Observation of the geometric phase effect in the H+HD -> H-2+D reaction below the conical intersection".Nature Communications 11.1(2020).