A Neural Network Potential Energy Surface and Quantum Dynamics Study of Ca(1S) + H2(v 0 = 0, j 0 = 0) → CaH + H Reaction.

Abstract

The reactive collision between Ca and H2 molecules has attracted great interest experimentally due to the key role of the product CaH molecule in the field of astrophysics and cold molecules. However, quantum dynamics calculations for this system have not been reported due to the lack of a global potential energy surface (PES). Herein, a globally accurate PES of the ground-state CaH2 is developed by combining 11365 high-level ab initio points and permutation invariant polynomial neural network method. Based on the newly constructed PES, the state-to-state quantum dynamics calculations for the Ca(1S) + H2 (v 0 = 0, j 0 = 0) → CaH + H reaction are carried out using the time-dependent wave packet method. The dynamic results reveal that the reaction follows the complex-forming mechanism near the reactive threshold, whereas both the indirect insertion mechanism and direct abstraction mechanism have effects at higher collision energies. The newly constructed PES can be used to further study the influence of isotope substitution, rovibrational excitation, and spatial orientation of reactant molecules on reaction dynamics.