Yang Zijiang, Chen Hanghang, Mao Ye, Chen Maodu
Key Laboratory of Materials Modification by Laser, Electron, and Ion Beams (Ministry of Education), School of Physics, Dalian University of Technology, Dalian 116024, P. R. China.
Phys Chem Chem Phys. 2022 Aug 17;24(32):19209-19217. doi: 10.1039/d2cp02711a.
Reactive collisions of Ca ions with H 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 CaH is constructed using the permutation invariant polynomial neural network method based on 27 780 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(S) + H( = 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.
钙离子与氢分子的反应性碰撞在超冷化学、量子信息及其他前沿领域中起着至关重要的作用，并且已经得到了广泛的实验研究，但由于缺乏适用的势能面（PES），相应的理论研究尚未见报道。在此，基于在多参考组态相互作用水平下计算得到的27780个点，采用置换不变多项式神经网络方法构建了基态CaH的全局精确PES。在新的PES上，进行了量子含时波包计算以研究Ca(S) + H( = 0, = 0) → CaH + H反应的动力学机制。计算结果表明，当碰撞能量低于5.0 eV时，该反应遵循直接提取过程。动力学结果对于该反应体系在更精细水平上的实验研究具有重要的参考意义，并且可以在这个新构建的PES上开展进一步的动力学研究，如同位素取代和反应物分子的振转激发的影响。
