Direct Observation of the C + S-2 Channel in CS2 Photodissociation

Li, Zhenxing1,2; Zhao, Min1,2; Xie, Ting1,2; Luo, Zijie3; Chang, Yao3; Cheng, Gongkui3; Yang, Jiayue3; Chen, Zhichao3; Zhang, Weiqing3; Wu, Guorong3; Wang, Xingan1,2; Yuan, Kaijun3; Yang, Xueming3,4

2021-01-21

10.1021/acs.jpclett.0c03386

Journal of Physical Chemistry Letters   影响因子和分区

1948-7185

Carbon disulfide (CS2) is a typical triatomic molecule. Its photodissociation process has generally been assumed to proceed to CS and S primary products via single bond fission. However, recent theoretical calculations suggested that an exit channel to produce C + S-2 should also be energetically accessible. Her; we report the direct experimental evidence for the C + S-2 channel in CS2 photodissociation by using the velocity map ion imaging technique with two-photon UV and one-photon vacuum (VUV) excitations. The detection of the C (P-3) products illustrates that the ground state and the electronically excited states of S-2 coproducts are formed within highly excited vibrational states. The very weak anisotropic distributions indicate relatively slow dissociation processes. The possible dissociation mechanism involves molecular isomerization of CS2 to linear-CSS from the excited B-1(2) (2(1)Sigma(+)) state via vibronic coupling with the in state followed by an avoided crossing with the ground state surface. Our results imply that the S-2 molecules observed in comets might be primarily formed in CS2 photodissociation.

SCI ; EI

英语

NI论文

通讯

Chemical Dynamics Research Center[21688102] ; National Natural Science Foundation of China (NSFC)[21873099,21922306,21590802] ; Key Technology Team of the Chinese Academy of Sciences[GJJSTD20190002] ; international partnership program of Chinese Academy of Sciences[121421KYSB20170012] ; Strategic Priority Research Program of the Chinese Academy of Sciences[XDB17000000]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Atomic, Molecular & Chemical

WOS:000613200600018

AMER CHEMICAL SOC

20210509846392

Ground state ; Imaging techniques ; Isomers ; Molecules ; Photodissociation ; Photons ; Sulfur compounds

Imaging Techniques:746 ; Physical Chemistry:801.4 ; Chemical Products Generally:804 ; Atomic and Molecular Physics:931.3

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.Southern Univ Sci & Technol, Coll Sci, Dept Chem, Shenzhen 518055, Peoples R China

Li, Zhenxing,Zhao, Min,Xie, Ting,et al. Direct Observation of the C + S-2 Channel in CS2 Photodissociation[J]. Journal of Physical Chemistry Letters,2021,12(2):844-849.

Li, Zhenxing.,Zhao, Min.,Xie, Ting.,Luo, Zijie.,Chang, Yao.,...&Yang, Xueming.(2021).Direct Observation of the C + S-2 Channel in CS2 Photodissociation.Journal of Physical Chemistry Letters,12(2),844-849.

Li, Zhenxing,et al."Direct Observation of the C + S-2 Channel in CS2 Photodissociation".Journal of Physical Chemistry Letters 12.2(2021):844-849.