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

IF 4.6 Q2 MATERIALS SCIENCE, BIOMATERIALS

ACS Applied Bio Materials Pub Date : 2024-10-23 DOI:10.1021/acs.jpca.4c0571210.1021/acs.jpca.4c05712

Jiapeng Zhang, Bayaer Buren* and Yongqing Li*,

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Abstract

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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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

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。

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来源期刊

ACS Applied Bio Materials Chemistry-Chemistry (all)

CiteScore

9.40

自引率

2.10%

发文量

464