Efficient Energy Transfer in Light-Harvesting Systems, III: The Influence of the Eighth Bacteriochlorophyll on the Dynamics and Efficiency in FMO

被引:133
作者
Moix, Jeremy [1 ,2 ,5 ]
Wu, Jianlan [3 ]
Huo, Pengfei [4 ]
Coker, David [4 ,6 ,7 ]
Cao, Jianshu [1 ,5 ]
机构
[1] MIT, Dept Chem, Cambridge, MA 02139 USA
[2] Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore
[3] Zhejiang Univ, Dept Phys, Hangzhou 310027, Peoples R China
[4] Boston Univ, Dept Chem, Boston, MA 02215 USA
[5] Singapore MIT Alliance Res & Technol, Singapore 117456, Singapore
[6] Univ Coll Dublin, Complex Adapt Syst Lab, Dublin 4, Ireland
[7] Univ Coll Dublin, Sch Phys, Dublin 4, Ireland
基金
美国国家科学基金会; 爱尔兰科学基金会;
关键词
PHYSIOLOGICAL TEMPERATURE; QUANTUM COHERENCE; PHOTOSYNTHETIC SYSTEM; PROTEIN; SPECTROSCOPY; BATH;
D O I
10.1021/jz201259v
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The most recent crystal structure of the Fenna-Matthews-Olson (FMO) protein complex indicates the presence of an additional eighth chromophore, which has been proposed to serve as a link between the chlorosome and the remaining seven chromophores. Here, we investigate the implications of this scenario through numerical calculations with the generalized Bloch-Redfield (GBR) equation and the noninteracting blip approximation (NIBA). It is shown that the oscillations often observed in the population relaxation of sites 1 and 2 may be completely suppressed in the eight-site model due to the initial preparation. Second it is demonstrated that while the presence of the eighth chromophore does not cause a dramatic change in the energy-transfer efficiency, it does however lead to a dominant energy-transfer pathway that can be characterized by an effective three-site system. Finally, we confirm that the energy-transfer process in the eight-site complex remains efficient and robust through computations of the optimal values of the bath parameters.
引用
收藏
页码:3045 / 3052
页数:8
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