基于神经网络势能面的 Na + Na2 交换反应量子动力学研究及 Na3 复合物寿命预测

IF 2.7 2区 化学 Q3 CHEMISTRY, PHYSICAL
Jiapeng Zhang, Bayaer Buren* and Yongqing Li*, 
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引用次数: 0

摘要

基于高水平的 ab initio 计算和基本不变神经网络 (FI-NN) 方法,构建了 Na3 体系的高精度全局势能面 (PES)。PES 的均方根误差 (RMSE) 为 2.88 cm-1。在新的 PES 上使用时间相关波包 (TDWP) 方法研究了基态 Na + Na2 (v = 0, j = 0) → Na2 (v′, j′) + Na 反应的状态分辨量子动力学。对相关积分截面的分析揭示了碰撞过程中复杂的能量传递机制。同样,微分截面的特征也表明复合物形成机制在反应中起着主导作用,这为全面探索复合物的寿命提供了条件。根据 Rice-Ramsperger-Kassel-Marcus (RRKM) 理论,计算出 Na3 复合物的寿命约为 3.9 ns。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Study on Quantum Dynamics of the Na + Na2 Exchanged Reaction and Lifetime Prediction of Na3 Complex Based on the Neural Network Potential Energy Surface

Study on Quantum Dynamics of the Na + Na2 Exchanged Reaction and Lifetime Prediction of Na3 Complex Based on the Neural Network Potential Energy Surface

A high-precision global potential energy surface (PES) is constructed for the Na3 system based on high-level ab initio calculations and the fundamental invariant neural network (FI-NN) method. The root-mean-square error (RMSE) of the PES is 2.88 cm–1. The state-resolved quantum dynamics of the ground-state Na + Na2 (v = 0, j = 0) → Na2 (v′, j′) + Na reaction is studied using the time-dependent wave packet (TDWP) method on the new PES. Analysis of the relevant integral cross sections revealed a complicated energy-transfer mechanism during collisions. Similarly, the characteristics of the differential cross sections indicate that the complex-forming mechanism plays a dominant role in the reaction, providing conditions for a comprehensive exploration of the lifetimes of the complexes. Based on the Rice-Ramsperger-Kassel-Marcus (RRKM) theory, the calculated lifetime of the Na3 complex is approximately 3.9 ns.

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来源期刊
The Journal of Physical Chemistry A
The Journal of Physical Chemistry A 化学-物理:原子、分子和化学物理
CiteScore
5.20
自引率
10.30%
发文量
922
审稿时长
1.3 months
期刊介绍: The Journal of Physical Chemistry A is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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