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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >H-Atom Product Channel in the Ultraviolet Photodissociation of the Thiomethoxy Radical (CH3S) via the (B)over-tilde(2)A(2) State
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H-Atom Product Channel in the Ultraviolet Photodissociation of the Thiomethoxy Radical (CH3S) via the (B)over-tilde(2)A(2) State

机译：H-原子产品通道在紫外线光积极的巯基甲氧基团（CH3S）通过（b）过褶（2）A（2）状态

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摘要

The photodissociation dynamics of jet-cooled thiomethoxy radical (CH3S) via the (B) over tilde (2)A(2) <- (X) over tilde E-2 transition was studied in the ultraviolet region of 216-225 nm using the high-n Rydberg H-atom time-of-flight (HRTOF) technique. The H-atom product channel was directly observed from the H-atom TOF spectra (using both dimethyl disulfide and dimethyl sulfide precursors). The H-atom photofragment yield spectrum showed a broad feature in the region of 216-225 nm and three (B) over tilde (2)A(2) vibronic peaks at 217.7, 220.3, and 221.5 nm. Several H-atom dissociation pathways were identified. The excited-state CH3S had a repulsive, prompt dissociation pathway to the ground-state H2CS((X) over tilde (1)A(1)) + H products, with the product translational energy peaking near the maximum available energy, a predominant C-S stretch vibrational excitation in H2CS((X) over tilde (1)A(1)), and an anisotropic angular distribution. The main pathway was the H2CS((X) over tilde (1)A(1)) + H product channel via the unimolecular dissociation of internally hot CH3S radical in the ground electronic state after internal conversion from the electronic excited state, with a modest translational energy release (peaking at a low translational energy of similar to 11 kcal/mol and extending near the maximum available energy) and a nearly isotropic angular distribution. The H + H2CS((A) over tilde (1)A(2)) and H + H2CS((a) over tilde (3)A(2)) product channels were also observed but were minor channels. The C-H bond dissociation energy of CH3S to the H + H2CS((X) over tilde (1)A(1)) products was determined to be 48.8 +/- 0.7 kcal/mol.
机译：在使用紫外线区域的紫外线区域中研究了通过（b）通过（b）替氏卵石E-2转变的喷射冷却硫氧基氧基自由基（CH3s）的光析和动态。在216-225nm的紫外线区域中研究了高N rydberg H-Atom飞行时间（HRTOF）技术。从H-Atom TOF光谱直接观察H-原子产品通道（使用二甲基二硫化物和二甲基硫醚前体）。 H-Atom PhotoFragment Exiting谱显示在216-225nm和三（b）的区域中，在217.7,220.3和221.5nm处的Tilde（2）A（2）振动峰的宽特征。确定了几种H-原子解离途径。激发态CH3s对地面H2Cs（（x）通过扭矩（1）A（1））+ H产品具有令人厌恶的及时解离途径，其产品平移能量达到最大可用能量，主要是峰值CS在TildE（1）A（1）上的H 2 Cs（（x）中拉伸振动激发，以及各向异性角度分布。主要途径是TildE（（1）A（1）A（1））+ H产品通道的H2Cs（（x），通过在从电子激发态的内部转换后的地面电子状态下的内部热的CH3s自主分离，具有谦虚平移能量释放（在低平移能量下达到相似的11kcal / mol，并且在最大可用能量附近延伸）和近各向同性的角度分布。还观察到H + H 2 C（（a）折叠式（1）A（2））和H + H 2C（（a）（3）A（2））产品通道，但是是小通道。将CH3键与H + H 2 Cs（（x）替换Tilde（1）A（1））产物的C-H键离解离能量测定为48.8 +/- 0.7kcal / mol。

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