Rotational and nuclear-spin level dependent photodissociation dynamics of H2S

Yarui Zhao, Zijie Luo, Yao Chang, Yucheng Wu, Su-e Zhang, Zhenxing Li, Hongbin Ding, Guorong Wu, Jyoti S. Campbell, Christopher S. Hansen (), Stuart W. Crane, Colin M. Western, Michael N. R. Ashfold (), Kaijun Yuan () and Xueming Yang
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Yarui Zhao: Dalian University of Technology
Zijie Luo: Chinese Academy of Sciences
Yao Chang: Chinese Academy of Sciences
Yucheng Wu: Chinese Academy of Sciences
Su-e Zhang: Chinese Academy of Sciences
Zhenxing Li: Chinese Academy of Sciences
Hongbin Ding: Dalian University of Technology
Guorong Wu: Chinese Academy of Sciences
Jyoti S. Campbell: University of New South Wales
Christopher S. Hansen: University of New South Wales
Stuart W. Crane: University of Bristol
Colin M. Western: University of Bristol
Michael N. R. Ashfold: University of Bristol
Kaijun Yuan: Chinese Academy of Sciences
Xueming Yang: Chinese Academy of Sciences

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract The detailed features of molecular photochemistry are key to understanding chemical processes enabled by non-adiabatic transitions between potential energy surfaces. But even in a small molecule like hydrogen sulphide (H2S), the influence of non-adiabatic transitions is not yet well understood. Here we report high resolution translational spectroscopy measurements of the H and S(1D) photoproducts formed following excitation of H2S to selected quantum levels of a Rydberg state with 1B1 electronic symmetry at wavelengths λ ~ 139.1 nm, revealing rich photofragmentation dynamics. Analysis reveals formation of SH(X), SH(A), S(3P) and H2 co-fragments, and in the diatomic products, inverted internal state population distributions. These nuclear dynamics are rationalised in terms of vibronic and rotational dependent predissociations, with relative probabilities depending on the parent quantum level. The study suggests likely formation routes for the S atoms attributed to solar photolysis of H2S in the coma of comets like C/1995 O1 and C/2014 Q2.

Date: 2021
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DOI: 10.1038/s41467-021-24782-6

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