{"title":"对撞能量为 266.2 和 206.5 cm-1 时 S(1D) + D2 → SD(2Π3/2,1/2) + D 反应的实验自旋轨道态分辨差分截面。","authors":"Yu Li, Heilong Wang, Zhirun Jiao, Hongtao Zhang, Bingbing Zhang, Xingan Wang, Chunlei Xiao, Xueming Yang","doi":"10.1021/acs.jpca.4c06605","DOIUrl":null,"url":null,"abstract":"<p><p>The S(<sup>1</sup>D) + D<sub>2</sub> → SD + D reaction is a prototype insertion chemical reaction that involves spin-orbit interactions in the exit channel. In this work, we report spin-orbit state-resolved differential cross sections (DCSs) of this reaction obtained by crossed beam experiments at collision energies of 266.2 and 206.5 cm<sup>-1</sup>. The DCSs of specific rovibrational states exhibit a slight preference for forward scattering. When integrated over all rotational quantum states within each spin-orbit manifold, the total angular distributions of the two manifolds show nearly forward-backward symmetry, indicating that the deep well responsible for the long-living complex-forming mechanism predominates the entire reaction dynamics. Moreover, significant spin-orbit preference was observed at rotational quantum number <i>N</i> > 9 in the vibrationally ground state of SD products. It was also observed that SD products in the vibrationally excited state <i>v</i>' = 1 prefer to populate in the <sup>2</sup>Π<sub>3/2</sub> manifold, with the <sup>2</sup>Π<sub>3/2</sub>/<sup>2</sup>Π<sub>1/2</sub> ratio of 15.8 and 25.2 at collision energies of 266.2 and 206.5 cm<sup>-1</sup>, respectively. The experimental spin-orbit state-resolved DCSs obtained in this work will be of great importance for developing an accurate diabatic theory that includes spin-orbit interactions for this title reaction.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":" ","pages":"10234-10239"},"PeriodicalIF":2.7000,"publicationDate":"2024-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Experimental Spin-Orbit State-Resolved Differential Cross Sections of the S(<sup>1</sup>D) + D<sub>2</sub> → SD(<sup>2</sup>Π<sub>3/2,1/2</sub>) + D Reaction at Collision Energies of 266.2 and 206.5 cm<sup>-1</sup>.\",\"authors\":\"Yu Li, Heilong Wang, Zhirun Jiao, Hongtao Zhang, Bingbing Zhang, Xingan Wang, Chunlei Xiao, Xueming Yang\",\"doi\":\"10.1021/acs.jpca.4c06605\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>The S(<sup>1</sup>D) + D<sub>2</sub> → SD + D reaction is a prototype insertion chemical reaction that involves spin-orbit interactions in the exit channel. In this work, we report spin-orbit state-resolved differential cross sections (DCSs) of this reaction obtained by crossed beam experiments at collision energies of 266.2 and 206.5 cm<sup>-1</sup>. The DCSs of specific rovibrational states exhibit a slight preference for forward scattering. When integrated over all rotational quantum states within each spin-orbit manifold, the total angular distributions of the two manifolds show nearly forward-backward symmetry, indicating that the deep well responsible for the long-living complex-forming mechanism predominates the entire reaction dynamics. Moreover, significant spin-orbit preference was observed at rotational quantum number <i>N</i> > 9 in the vibrationally ground state of SD products. It was also observed that SD products in the vibrationally excited state <i>v</i>' = 1 prefer to populate in the <sup>2</sup>Π<sub>3/2</sub> manifold, with the <sup>2</sup>Π<sub>3/2</sub>/<sup>2</sup>Π<sub>1/2</sub> ratio of 15.8 and 25.2 at collision energies of 266.2 and 206.5 cm<sup>-1</sup>, respectively. The experimental spin-orbit state-resolved DCSs obtained in this work will be of great importance for developing an accurate diabatic theory that includes spin-orbit interactions for this title reaction.</p>\",\"PeriodicalId\":59,\"journal\":{\"name\":\"The Journal of Physical Chemistry A\",\"volume\":\" \",\"pages\":\"10234-10239\"},\"PeriodicalIF\":2.7000,\"publicationDate\":\"2024-11-28\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"The Journal of Physical Chemistry A\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.jpca.4c06605\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/11/18 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry A","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.jpca.4c06605","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/11/18 0:00:00","PubModel":"Epub","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Experimental Spin-Orbit State-Resolved Differential Cross Sections of the S(1D) + D2 → SD(2Π3/2,1/2) + D Reaction at Collision Energies of 266.2 and 206.5 cm-1.
The S(1D) + D2 → SD + D reaction is a prototype insertion chemical reaction that involves spin-orbit interactions in the exit channel. In this work, we report spin-orbit state-resolved differential cross sections (DCSs) of this reaction obtained by crossed beam experiments at collision energies of 266.2 and 206.5 cm-1. The DCSs of specific rovibrational states exhibit a slight preference for forward scattering. When integrated over all rotational quantum states within each spin-orbit manifold, the total angular distributions of the two manifolds show nearly forward-backward symmetry, indicating that the deep well responsible for the long-living complex-forming mechanism predominates the entire reaction dynamics. Moreover, significant spin-orbit preference was observed at rotational quantum number N > 9 in the vibrationally ground state of SD products. It was also observed that SD products in the vibrationally excited state v' = 1 prefer to populate in the 2Π3/2 manifold, with the 2Π3/2/2Π1/2 ratio of 15.8 and 25.2 at collision energies of 266.2 and 206.5 cm-1, respectively. The experimental spin-orbit state-resolved DCSs obtained in this work will be of great importance for developing an accurate diabatic theory that includes spin-orbit interactions for this title reaction.
期刊介绍:
The Journal of Physical Chemistry A is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.