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飞秒激发下光合反应中心中的电荷分离

Charge separation in photosynthetic reaction centers under femtosecond excitation.

作者信息

Yakovlev A G, Shuvalov V A

机构信息

Belozersky Institute of Physico-Chemical Biology, Lomonosov Moscow State University, Moscow, 119899, Russia.

出版信息

Biochemistry (Mosc). 2001 Feb;66(2):211-20. doi: 10.1023/a:1002851817005.

Abstract

The process of electron transfer from the primary electron donor P* to the primary electron acceptor BA in the reaction center of Rhodobacter sphaeroides R-26 under 30 fsec pulse excitation was studied in this work with the aim of establishing a relationship between the nuclear subsystem motion and charge transfer. For this purpose the fsec and psec oscillations in the bands of stimulated emission of P* and in the band of reaction product BA- at 1020 nm were investigated. It was established that the reversible formation of the P+BA- state is characterized by two vibration modes (130 and 320 cm(-1)) and connected with an arrival of the wavepacket induced by fsec excitation to the intersection of potential surfaces P*BA and P+BA-. The irreversible formation of the P+BA- state with the time constant of 3 psec is followed by oscillations with frequencies of 9 and 33 cm(-1). These results show that the irreversibility of electron transfer is determined by two factors: 1) by a difference between the energy width of the wavepacket and the gap between the named surfaces; 2) by a difference between the duration of wavepacket residence near the intersection of the surfaces and the relaxation time of the P+BA- state.

摘要

本研究通过在30飞秒脉冲激发下,对球形红杆菌R-26反应中心中从初级电子供体P到初级电子受体BA的电子转移过程进行研究,旨在建立核子系统运动与电荷转移之间的关系。为此,研究了P受激发射带以及1020nm处反应产物BA-带中的飞秒和皮秒振荡。结果表明,P+BA-态的可逆形成具有两种振动模式(130和320cm-1),并与飞秒激发诱导的波包到达势能面P*BA和P+BA-的交点有关。P+BA-态以3皮秒的时间常数不可逆形成,随后出现频率为9和33cm-1的振荡。这些结果表明,电子转移的不可逆性由两个因素决定:1)波包能量宽度与上述表面之间能隙的差异;2)波包在表面交点附近的停留时间与P+BA-态弛豫时间的差异。

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