类胡萝卜素新的暗激发态在光合作用体系中的作用
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- 英文论文题名：New Dark Excited State of Carotenoids in Photosynthesic Complex
- 论文作者：冯瑾 ; 马玉臣
- 英文论文作者：Jin Feng ; Yuchen Ma ; School of Chemistry and Chemical Engineering ; Shandong University
- 年：2016
- 作者机构：山东大学化学与化工学院;
- 论文关键词：类胡萝卜素 ; 叶绿素 ; 能量传递 ; 中间态
- 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-第十八分会：电子结构理论方法的发展与应用
- 语种：中文
- 分类号：O629.4
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第十八分会 ; 电子结构理论方法的发展与应用
- 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：319k
- 原文格式：D
- 会议级别：全国
摘要
大量实验和计算发现在自然光合系统中,除了原始的三段论(S_0-S_2-S_1-S_0)之外,S_2和S_1之间存在新的暗态。但关于新态的特征和起源,仍存在着很多争议。我们通过第一性的多体格林函数理论和能量传递理论的计算,发现了新态S_y。它是在S_2弛豫过程中可到达的单激发态,而不是被大家一直争议的双激发1Bu~-或者3Ag~-态。我们通过激发态优化,进一步证实,通过非辐射跃迁可以实现S_2到S_y的能量传递。我们还进一步研究了类胡萝卜素和叶绿素之间以及叶绿素之间的能量传递。我们的计算结果很好地解释了近期二维电子光谱实验对各种光合作用体系的测量结果。
It has been generally accepted that an intermediate state mediates the energy transfer process from carotenoid to chlorophyll in natural light-harvesting systems.However, there is still much controversy on the origin and characteristics of the intermediate state.By ab initio many-body Green's function theory, together with the F?rster-Dexter theory, we identify a new dark singlet excited state(deonoted as S_y), which is accessible from the S_2 state at the optical absorption maximum via nonadiabatic transition, that may play the role of the intermediate state.S_y is composed by singly excited configurations, which is different from the general assignment of the intemediate state to states 1Bu~-and/or 3Ag~-formed by double excitations.The closeness of the potential minimum between states S_y and S_2 in energy is a general feature for long polyene chains.
It has been generally accepted that an intermediate state mediates the energy transfer process from carotenoid to chlorophyll in natural light-harvesting systems.However, there is still much controversy on the origin and characteristics of the intermediate state.By ab initio many-body Green's function theory, together with the F?rster-Dexter theory, we identify a new dark singlet excited state(deonoted as S_y), which is accessible from the S_2 state at the optical absorption maximum via nonadiabatic transition, that may play the role of the intermediate state.S_y is composed by singly excited configurations, which is different from the general assignment of the intemediate state to states 1Bu~-and/or 3Ag~-formed by double excitations.The closeness of the potential minimum between states S_y and S_2 in energy is a general feature for long polyene chains.
引文
[1]Ostroumov,E.E.;Mulvaney,R.M.;Cogdell,R.J.;Scholes,G.D.Science.2013,340:52.
[2]Ostroumov,E.;Müller,M.G.;Marian,C.M.;Kleinschmidt,M.;Holzwarth,A.R.Phys.Rev.Lett.2009,103:108302.
[2]Ostroumov,E.;Müller,M.G.;Marian,C.M.;Kleinschmidt,M.;Holzwarth,A.R.Phys.Rev.Lett.2009,103:108302.