An ab initio-based global potential energy surface for the SH3 system and full-dimensional state-to-state quantum dynamics study for the H2 + HS → H2S + H reaction
An ab initio-based global potential energy surface for the SH3 system and full-dimensional state-to-state quantum dynamics study for the H2 + HS → H2S + H reaction
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SH3 系统的从头算全局势能面和 H2 HS — H2S H 反应的全维态到态量子动力学研究
DOI：
10.1002/jcc.25746
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发表时间：
2019
影响因子：
3
通讯作者：
Zhang Dong H
中科院分区：
文献类型：
--
作者：
Xu Xin;Chen Jun;Liu Shu;Zhang Dong H
利用41882个高能级初能点和神经网络拟合方法，构建了SH3系统基态电子态的精确势能面。基于反应物-产物解耦方案，时间相关波包方法已用于计算全尺寸标题反应的第一个状态到状态微分截面，最高可达 1.2 eV。研究发现，大部分 H2S 是在基振动状态下产生的，反应的大部分可用能量最终以产物平移运动的形式产生。阈值能量处的微分横截面主要由向后方向上的非常窄的峰主导。随着碰撞能量的增加，角分布的宽度显着增加，这是抽象机制直接反应的典型特征，类似于H2+ OH→H2O + H反应。 © 2018 Wiley 期刊公司。
An accurate potential energy surface for the ground electronic state of SH3system has been constructed with 41,882 high levelab initioenergy points and the neural network fitting method. The time‐dependent wave packet method has been used to calculate the first state‐to‐state differential cross sections for the title reaction up to 1.2 eV in full dimensions, based on the reactant–product decoupling scheme. It is found that the majority of H2S are produced in the ground vibrational state, with a large fraction of available energy for the reaction ending up as product translational motion. The differential cross sections at the threshold energy are dominated by a very narrow peak in the backward direction. With the increase of collision energy, the width of the angular distribution increases considerably, which is a typical feature of a direct reaction via abstract mechanism, similar to the H2+ OH → H2O + H reaction. © 2018 Wiley Periodicals, Inc.