A neural network potential energy surface and quantum dynamics studies for the Ca+(2S) + H2 → CaH+ + H reaction. Issue 32 (3rd August 2022)

• Record Type: Journal Article
• Authors: Yang, Zijiang; Chen, Hanghang; Mao, Ye; Chen, Maodu
• Is Part Of: Physical chemistry chemical physics. Volume 24:Issue 32(2022)
• Page Start: 19209
• Page End: 19217
• Publication Date: 2022-08-03
• Subjects: Chemistry, Physical and theoretical -- Periodicals; 541.3
• DOI: 10.1039/d2cp02711a
• Languages: English
• ISSNs: 1463-9076

Abstract

Abstract : A globally accurate PES and dynamics studies for the Ca + ( 2 S) + H2 → CaH + + H reaction. Abstract : Reactive collisions of Ca + ions with H2 molecules play a crucial role in ultracold chemistry, quantum information and other cutting-edge fields, and have been widely studied experimentally, but the corresponding theoretical studies have not been reported due to the lack of an applicable potential energy surface (PES). Herein, a globally accurate PES of the ground-state CaH2 + is constructed using the permutation invariant polynomial neural network method based on 27 780 ab initio points calculated at the multi-reference configuration interaction level. On the new PES, the quantum time-dependent wave packet calculations are performed to study the dynamics mechanisms of the Ca + ( 2 S) + H2 ( ν 0 = 0, j 0 = 0) → CaH + + H reaction. The calculated results suggest that the reaction follows a direct abstraction process when the collision energy is below 5.0 eV. The dynamics results would have a great reference significance for the experimental research of this reactive system at a finer level, and further dynamics studies, such as the effects of isotope substitution and rovibrational excitations of the reactant molecule, could be carried out on this newly constructed PES.