Liu Siwen, Cheng Huiying, Cao Furong, Sun Jingchang, Yang Zijiang
School of Physics and Electronic Technology, Liaoning Normal University, Dalian 116029, China.
Molecules. 2024 Oct 14;29(20):4871. doi: 10.3390/molecules29204871.
The collisions between Na atoms and H molecules are of great significance in the field of chemical reaction dynamics, but the corresponding dynamics results of ground-state reactions have not been reported experimentally or theoretically. Herein, a global and high-precision potential energy surface (PES) of NaH (1') is constructed by the neural network model based on 21,873 high-level ab initio points. On the newly constructed PES, the quantum dynamics calculations on the Na(S) + H( = 0, = 0) → NaH + H reaction are carried out using the time-dependent wave packet method to study the microscopic reaction mechanism at the state-to-state level. The calculated results show that the low-vibrational products are mainly formed by the dissociation of the triatomic complex; whereas, the direct reaction process dominates the generation of the products with high-vibrational states. The reaction generally follows the direct H-abstraction process, and there is also the short-lived complex-forming mechanism that occurs when the collision energy exceeds the reaction threshold slightly. The PES could be used to further study the stereodynamics effects of isotope substitution and rovibrational excitations on the title reaction, and the presented dynamics data would provide an important reference on the corresponding experimental research at a higher level.
钠原子与氢分子之间的碰撞在化学反应动力学领域具有重要意义，但基态反应的相应动力学结果尚未有实验或理论报道。在此，基于21873个高水平从头算点，通过神经网络模型构建了NaH（1'）的全局高精度势能面（PES）。在新构建的PES上，采用含时波包方法对Na(S)+H( = 0, = 0)→NaH + H反应进行量子动力学计算，以研究态-态水平的微观反应机理。计算结果表明，低振动产物主要由三原子复合物的解离形成；而高振动态产物的生成则以直接反应过程为主导。该反应一般遵循直接氢提取过程，当碰撞能量略超过反应阈值时，还会出现短暂的复合物形成机制。该PES可用于进一步研究同位素取代和振转激发对标题反应的立体动力学效应，所呈现的动力学数据将为更高水平的相应实验研究提供重要参考。
