非绝热动力学多态轨线方法
详细信息 查看官网全文
- 英文论文题名：Multistate Trajectory Approach for Nonadiabatic Dynamics
- 论文作者：陶国华
- 英文论文作者：Guohua Tao ; Peking University Shenzhen Graduate School ; Shenzhen Key Laboratory of New Energy Materials by Design ; Peking University
- 年：2016
- 作者机构：北京大学深圳研究生院;北京大学深圳市新能源材料人工设计重点实验室;
- 论文关键词：非绝热动力学 ; 分子动力学模拟 ; 量子动力学
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第十九分会：化学中的量子与经典动力学
- 语种：中文
- 分类号：O561
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第十九分会 ; 化学中的量子与经典动力学
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：140k
- 原文格式：D
- 会议级别：全国
摘要
非绝热动力学在化学以及生物、材料等交叉领域中的很多关键分子过程中至关重要。实现原子尺度的非绝热动力学模拟可以为理解相关过程的微观机理构建分子模型提供直接有力的帮助。为实现实际体系非绝热分子动力学的精确有效模拟,我们开发了一种多态轨线方法[1]。该方法基于Meyer-Miller电子态经典映射理论,提出描述原子核-电子耦合体系的多态轨线表示,通过对称窗口函数确定体系的电子态,而每个电子态由相应的运动轨线描述,整个体系的动力学过程由所有电子态对应轨线的集合来描述。相比较其他非绝热动力学方法(比如Ehrenfest,surface hopping等),多态轨线方法物理图像清晰,原则上对于每个电子态特定的动力学描述更准确,核-电子耦合处理自洽,方法经济有效,具有良好的数值稳定性和实用性。采用多态轨线方法的非绝热动力学模拟可以有效地处理复杂分子体系的动力学过程,比如动力电池材料磷酸铁锂体系中的电子耦合锂离子扩散[2]。新方法对于非绝热动力学过程具有普遍适用性。
Nonadiabatic dynamics plays a key role in many important molecular processes in chemistry, biology and materials. We proposed a multistate trajectory approach to perform nonadiabatic molecular dynamics simulation accurately and efficiently for realistic molecular systems. The new method proposed a multistate trajectory representation for coupled electron-nuclear dynamics, i.e. each state is assigned with an individual trajectory, the ensemble of which describes the overall nuclear-electron coupled dynamics of the system. The electronic state is determined by the symmetrical windowing function based on the Meyer-Miller model for electronic degrees of freedom. The approach not only provides a clear multi-state picture, but describes the coupled electronic-nuclear dynamics consistently and accurately. The implementation of this approach for realistic complex molecular systems demonstrates its high efficiency and excellent numerical stability.
Nonadiabatic dynamics plays a key role in many important molecular processes in chemistry, biology and materials. We proposed a multistate trajectory approach to perform nonadiabatic molecular dynamics simulation accurately and efficiently for realistic molecular systems. The new method proposed a multistate trajectory representation for coupled electron-nuclear dynamics, i.e. each state is assigned with an individual trajectory, the ensemble of which describes the overall nuclear-electron coupled dynamics of the system. The electronic state is determined by the symmetrical windowing function based on the Meyer-Miller model for electronic degrees of freedom. The approach not only provides a clear multi-state picture, but describes the coupled electronic-nuclear dynamics consistently and accurately. The implementation of this approach for realistic complex molecular systems demonstrates its high efficiency and excellent numerical stability.
引文
[1]Tao,G.J.Chem.Phys.2016,144:094108.
[2]Tao,G.J.Phys.Chem.C 2016,http://dx.doi.org/10.1021/acs.jpcc.5b12676.
[2]Tao,G.J.Phys.Chem.C 2016,http://dx.doi.org/10.1021/acs.jpcc.5b12676.
© 2004-2018 中国地质图书馆版权所有 京ICP备05064691号 京公网安备11010802017129号 地址：北京市海淀区学院路29号 邮编：100083 电话：办公室：(+86 10)66554848；文献借阅、咨询服务、科技查新：66554700 |