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. Issue 10 (28th December 2018)

• Record Type: Journal Article
• Authors: Xu, Xin; Chen, Jun; Liu, Shu; Zhang, Dong H.
• Other Names: Mo Yirong guestEditor.; Wu Wei guestEditor.; Cao Zexing guestEditor.
• Is Part Of: Journal of computational chemistry. Volume 40:Issue 10(2019)
• Page Start: 1151
• Page End: 1160
• Publication Date: 2018-12-28
• Subjects: potential energy surface -- differential cross sections -- H2 + SH -- quantum dynamics -- time‐dependent wave packet; Chemistry -- Data processing -- Periodicals; 542.85
• DOI: 10.1002/jcc.25746
• Languages: English
• ISSNs: 0192-8651

Abstract

Abstract : An accurate potential energy surface for the ground electronic state of SH3 system has been constructed with 41, 882 high level ab initio energy 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 H2 S 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 → H2 O + H reaction. © 2018 Wiley Periodicals, Inc. Abstract : The authors construct a potential energy surface for the ground electronic state of the SH3 system with high level ab initio energy points and the neural network fitting method. Based on this new potential energy surfaces, they report the first full‐dimensional (6D) state‐to‐state differential cross sections up to 1.2 eV from the ground rovibrational initial state, using the reactant–product decoupling scheme‐based time‐dependent wave packet method.