{"title":"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","authors":"Jiapeng Zhang, Bayaer Buren* and Yongqing Li*, ","doi":"10.1021/acs.jpca.4c0571210.1021/acs.jpca.4c05712","DOIUrl":null,"url":null,"abstract":"<p >A high-precision global potential energy surface (PES) is constructed for the Na<sub>3</sub> system based on high-level <i>ab initio</i> calculations and the fundamental invariant neural network (FI-NN) method. The root-mean-square error (RMSE) of the PES is 2.88 cm<sup>–1</sup>. The state-resolved quantum dynamics of the ground-state Na + Na<sub>2</sub> (<i>v</i> = 0, <i>j</i> = 0) → Na<sub>2</sub> (<i>v</i>′, <i>j</i>′) + 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 Na<sub>3</sub> complex is approximately 3.9 ns.</p>","PeriodicalId":2,"journal":{"name":"ACS Applied Bio Materials","volume":null,"pages":null},"PeriodicalIF":4.6000,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Study on Quantum Dynamics of the Na + Na2 Exchanged Reaction and Lifetime Prediction of Na3 Complex Based on the Neural Network Potential Energy Surface\",\"authors\":\"Jiapeng Zhang, Bayaer Buren* and Yongqing Li*, \",\"doi\":\"10.1021/acs.jpca.4c0571210.1021/acs.jpca.4c05712\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >A high-precision global potential energy surface (PES) is constructed for the Na<sub>3</sub> system based on high-level <i>ab initio</i> calculations and the fundamental invariant neural network (FI-NN) method. The root-mean-square error (RMSE) of the PES is 2.88 cm<sup>–1</sup>. The state-resolved quantum dynamics of the ground-state Na + Na<sub>2</sub> (<i>v</i> = 0, <i>j</i> = 0) → Na<sub>2</sub> (<i>v</i>′, <i>j</i>′) + 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 Na<sub>3</sub> complex is approximately 3.9 ns.</p>\",\"PeriodicalId\":2,\"journal\":{\"name\":\"ACS Applied Bio Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.6000,\"publicationDate\":\"2024-10-23\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Bio Materials\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.jpca.4c05712\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"MATERIALS SCIENCE, BIOMATERIALS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Bio Materials","FirstCategoryId":"1","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.jpca.4c05712","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"MATERIALS SCIENCE, BIOMATERIALS","Score":null,"Total":0}
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。
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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