Theoretical study of photoinduced proton coupled electron transfer reaction using the non-perturbative hierarchical equations of motion method

doi:10.1063/1.4982928

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	Theoretical study of photoinduced proton coupled electron transfer reaction using the non-perturbative hierarchical equations of motion method
	Song, Kai ; Shi, Qiang 1
刊名	JOURNAL OF CHEMICAL PHYSICS
	2017-05-14
卷号	146 期号:18
ISSN号	0021-9606
DOI	10.1063/1.4982928
英文摘要	Photoinduced proton coupled electron transfer (PCET) reactions, in which the charge transfer process is initiated by light absorption, are of special interest to both theoretical and experimental studies. In this work, by employing the non-perturbative hierarchical equation of motion method, we investigate several aspects of concerted photoinduced PCET based on an extended spin-boson model where the correlation between the electron and proton baths is considered explicitly. It is found that the vibrational relaxation on the donor state plays an important role in the initial stage of the non-equilibrium PCET dynamics after photon excitation, and the equilibrium rate dynamics is recovered at times longer than the vibrational relaxation time scale. The numerically exact results are compared with those obtained from the non-equilibrium Fermi's golden rule, which is found to be less accurate for the non-equilibrium dynamics in the case of large electronic couplings. The isotope effect in photoinduced PCET is also investigated, where the non-equilibrium dynamics and equilibrium rate dynamics show very different isotope effects. Published by AIP Publishing.
语种	英语
出版者	AMER INST PHYSICS
WOS记录号	WOS:000401368900011
内容类型	期刊论文
源URL	[http://ir.iccas.ac.cn/handle/121111/44953]
专题	中国科学院化学研究所
通讯作者	Shi, Qiang
作者单位	1.Chinese Acad Sci, Beijing Natl Lab Mol Sci, State Key Lab Struct Chem Unstable & Stable Speci, CAS Res Educ Ctr Excellence Mol Sci,Inst Chem, Beijing 100190, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式 GB/T 7714	Song, Kai,Shi, Qiang. Theoretical study of photoinduced proton coupled electron transfer reaction using the non-perturbative hierarchical equations of motion method[J]. JOURNAL OF CHEMICAL PHYSICS,2017,146(18).
APA	Song, Kai,&Shi, Qiang.(2017).Theoretical study of photoinduced proton coupled electron transfer reaction using the non-perturbative hierarchical equations of motion method.JOURNAL OF CHEMICAL PHYSICS,146(18).
MLA	Song, Kai,et al."Theoretical study of photoinduced proton coupled electron transfer reaction using the non-perturbative hierarchical equations of motion method".JOURNAL OF CHEMICAL PHYSICS 146.18(2017).