Calculation of Electron Transfer Rates Using Mixed Quantum Classical Approaches: Nonadiabatic Limit and Beyond

doi:10.1021/jp400462f

CORC > 化学研究所 > 中国科学院化学研究所

	Calculation of Electron Transfer Rates Using Mixed Quantum Classical Approaches: Nonadiabatic Limit and Beyond
	Xie, Weiwei; Bai, Shuming; Zhu, Lili; Shi, Qiang
刊名	JOURNAL OF PHYSICAL CHEMISTRY A
	2013-07-25
卷号	117 期号:29 页码:6196-6204
ISSN号	1089-5639
DOI	10.1021/jp400462f
英文摘要	We investigate the applicability of the Ehrenfest and surface hopping methods to calculate electron transfer rates using the spin-boson model with different parameters. Rate constants are obtained from short time dynamics performed in both the diabatic and adiabatic basis sets. Numerical results and theoretical analysis show that these two methods can be reasonably accurate in the nonadiabatic limit, by staying close to an approximate Fermi's golden rule. Beyond the nonadiabatic limit, the calculated mixed quantum classical rates are compared with numerical exact results, and similar accuracy was found as in the nonadiabatic limit. The relation between the current finding and recent studies using the surface hopping method based on long time dynamics is also discussed. It is found that the short time dynamics could be more accurate in calculating rate constants using the mixed quantum classical methods.
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000322503200035
内容类型	期刊论文
源URL	[http://ir.iccas.ac.cn/handle/121111/53717]
专题	中国科学院化学研究所
通讯作者	Shi, Qiang
作者单位	Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci, State Key Lab Struct Chem Unstable & Stable Speci, Beijing 100190, Peoples R China
推荐引用方式 GB/T 7714	Xie, Weiwei,Bai, Shuming,Zhu, Lili,et al. Calculation of Electron Transfer Rates Using Mixed Quantum Classical Approaches: Nonadiabatic Limit and Beyond[J]. JOURNAL OF PHYSICAL CHEMISTRY A,2013,117(29):6196-6204.
APA	Xie, Weiwei,Bai, Shuming,Zhu, Lili,&Shi, Qiang.(2013).Calculation of Electron Transfer Rates Using Mixed Quantum Classical Approaches: Nonadiabatic Limit and Beyond.JOURNAL OF PHYSICAL CHEMISTRY A,117(29),6196-6204.
MLA	Xie, Weiwei,et al."Calculation of Electron Transfer Rates Using Mixed Quantum Classical Approaches: Nonadiabatic Limit and Beyond".JOURNAL OF PHYSICAL CHEMISTRY A 117.29(2013):6196-6204.