The vibronic state dependent predissociation of H2S: determination of all fragmentation processes

Zhao, Yarui1,2; Chen, Junjie3; Luo, Zijie2; Chang, Yao2; Yang, Jiayue2; Zhang, Weiqing2; Wu, Guorong2; Crane, Stuart W.4; Hansen, Christopher S.5; Ding, Hongbin1; An, Feng3; Hu, Xixi6,7; Xie, Daiqian3,7; Ashfold, Michael N. R.4; Yuan, Kaijun2,7; Yang, Xueming2,7,8

2023-02-01

10.1039/d2sc06988a

Chemical Science   影响因子和分区

2041-6520

2041-6539

Photochemistry plays a significant role in shaping the chemical reaction network in the solar nebula and interstellar clouds. However, even in a simple triatomic molecule photodissociation, determination of all fragmentation processes is yet to be achieved. In this work, we present a comprehensive study of the photochemistry of H2S, derived from cutting-edge translational spectroscopy measurements of the H, S(D-1) and S(S-1) atom products formed by photolysis at wavelengths across the range 155-120 nm. The results provide detailed insights into the energy disposal in the SH(X), SH(A) and H-2 co-fragments, and the atomisation routes leading to two H atoms along with S(P-3) and S(D-1) atoms. Theoretical calculations allow the dynamics of all fragmentation processes, especially the bimodal internal energy distributions in the diatomic products, to be rationalised in terms of non-adiabatic transitions between potential energy surfaces of both (1)A ' and (1)A '' symmetry. The comprehensive picture of the wavelength-dependent (or vibronic state-dependent) photofragmentation behaviour of H2S will serve as a text-book example illustrating the importance of non-Born-Oppenheimer effects in molecular photochemistry, and the findings should be incorporated in future astrochemical modelling.

SCI ; EI

英语

NI论文

其他

National Natural Science Foundation of China (NSFC Center for Chemical Dynamics)[22288201] ; National Natural Science Foundation of China["22241304","22073042","22122302","22225303","22233003"] ; Key Technology Team of the Chinese Academy of Sciences[GJJSTD20220001] ; Innovation Program for Quantum Science and Technology[2021ZD0303304] ; Liaoning Revitalization Talents Program[XLYC1907154] ; Australian Research Council (ARC)[DE200100549] ; Engineering and Physical Sciences Research Council (EPSRC)[EP/L005913]

Chemistry

Chemistry, Multidisciplinary

WOS:000936185800001

ROYAL SOC CHEMISTRY

20230913657763

Photodissociation ; Photolysis ; Potential energy ; Quantum chemistry

Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Atomic and Molecular Physics:931.3

Web of Science

1.Dalian Univ Technol, Sch Phys, Key Lab Mat Modificat Laser Ion & Electron Beams, Chinese Minist Educ, Dalian 116024, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam & Dalian Coherent Li, Dalian 116023, Peoples R China
3.Nanjing Univ, Inst Theoret & Computat Chem, Sch Chem & Chem Engn, Key Lab Mesoscop Chem, Nanjing 210023, Peoples R China
4.Univ Bristol, Sch Chem, Bristol BS81TS, England
5.Univ New South Wales, Sch Chem, Sydney, NSW 2052, Australia
6.Nanjing Univ, Ctr Modern Anal, Inst Brain Sci, Kuang Yaming Honors Sch,Jiangsu Key Lab Vehicle Em, Nanjing 210023, Peoples R China
7.Hefei Natl Lab, Hefei 230088, Peoples R China
8.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China

Zhao, Yarui,Chen, Junjie,Luo, Zijie,et al. The vibronic state dependent predissociation of H2S: determination of all fragmentation processes[J]. Chemical Science,2023,14(10):2501-2517.

Zhao, Yarui.,Chen, Junjie.,Luo, Zijie.,Chang, Yao.,Yang, Jiayue.,...&Yang, Xueming.(2023).The vibronic state dependent predissociation of H2S: determination of all fragmentation processes.Chemical Science,14(10),2501-2517.

Zhao, Yarui,et al."The vibronic state dependent predissociation of H2S: determination of all fragmentation processes".Chemical Science 14.10(2023):2501-2517.