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Multichannel photodissociation dynamics in CS2 studied by ultrafast electron diffraction
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2022-06-08 , DOI: 10.1039/d2cp01268e Weronika O Razmus 1 , Kyle Acheson 2 , Philip Bucksbaum 3 , Martin Centurion 4 , Elio Champenois 3 , Ian Gabalski 3 , Matthias C Hoffman 5 , Andrew Howard 3 , Ming-Fu Lin 5 , Yusong Liu 6 , Pedro Nunes 4 , Sajib Saha 4 , Xiaozhe Shen 7 , Matthew Ware 3 , Emily M Warne 1 , Thomas Weinacht 6 , Kyle Wilkin 4 , Jie Yang 7 , Thomas J A Wolf 3 , Adam Kirrander 2 , Russell S Minns 1 , Ruaridh Forbes 5
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2022-06-08 , DOI: 10.1039/d2cp01268e Weronika O Razmus 1 , Kyle Acheson 2 , Philip Bucksbaum 3 , Martin Centurion 4 , Elio Champenois 3 , Ian Gabalski 3 , Matthias C Hoffman 5 , Andrew Howard 3 , Ming-Fu Lin 5 , Yusong Liu 6 , Pedro Nunes 4 , Sajib Saha 4 , Xiaozhe Shen 7 , Matthew Ware 3 , Emily M Warne 1 , Thomas Weinacht 6 , Kyle Wilkin 4 , Jie Yang 7 , Thomas J A Wolf 3 , Adam Kirrander 2 , Russell S Minns 1 , Ruaridh Forbes 5
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The structural dynamics of photoexcited gas-phase carbon disulfide (CS2) molecules are investigated using ultrafast electron diffraction. The dynamics were triggered by excitation of the optically bright 1B2(1Σu+) state by an ultraviolet femtosecond laser pulse centred at 200 nm. In accordance with previous studies, rapid vibrational motion facilitates a combination of internal conversion and intersystem crossing to lower-lying electronic states. Photodissociation via these electronic manifolds results in the production of CS fragments in the electronic ground state and dissociated singlet and triplet sulphur atoms. The structural dynamics are extracted from the experiment using a trajectory-fitting filtering approach, revealing the main characteristics of the singlet and triplet dissociation pathways. Finally, the effect of the time-resolution on the experimental signal is considered and an outlook to future experiments provided.
中文翻译：
通过超快电子衍射研究 CS2 中的多通道光解动力学
使用超快电子衍射研究了光激发气相二硫化碳 (CS 2 ) 分子的结构动力学。通过以 200 nm 为中心的紫外飞秒激光脉冲激发光学明亮的1 B 2 ( 1 Σ u + ) 状态来触发动力学。根据先前的研究，快速振动运动促进了内部转换和系统间交叉到较低电子态的组合。光解通过这些电子流形导致产生电子基态的 CS 碎片和解离的单重态和三重态硫原子。使用轨迹拟合过滤方法从实验中提取结构动力学，揭示单线态和三线态解离途径的主要特征。最后，考虑了时间分辨率对实验信号的影响，并对未来的实验进行了展望。
更新日期：2022-06-08
中文翻译：
通过超快电子衍射研究 CS2 中的多通道光解动力学
使用超快电子衍射研究了光激发气相二硫化碳 (CS 2 ) 分子的结构动力学。通过以 200 nm 为中心的紫外飞秒激光脉冲激发光学明亮的1 B 2 ( 1 Σ u + ) 状态来触发动力学。根据先前的研究，快速振动运动促进了内部转换和系统间交叉到较低电子态的组合。光解通过这些电子流形导致产生电子基态的 CS 碎片和解离的单重态和三重态硫原子。使用轨迹拟合过滤方法从实验中提取结构动力学，揭示单线态和三线态解离途径的主要特征。最后，考虑了时间分辨率对实验信号的影响，并对未来的实验进行了展望。
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