Energy transfer in photosystem I of cyanobacteria Synechococcus elongatus: model study with structure-based semi-empirical Hamiltonian and experimental spectral density.
Energy transfer in photosystem I of cyanobacteria Synechococcus elongatus: model study with structure-based semi-empirical Hamiltonian and experimental spectral density.
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蓝藻细长聚球藻光系统 I 中的能量转移：基于结构的半经验哈密顿量和实验光谱密度的模型研究。
DOI：
10.1016/s0006-3495(03)74461-0
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发表时间：
2003
影响因子：
3.4
通讯作者：
G. Fleming
中科院分区：
文献类型：
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作者：
Mino Yang;Ana Damjanovic;Harsha M. Vaswani;G. Fleming
我们对 PSI 中的能量转移和捕获动力学进行建模。我们不是简单地应用福斯特理论，而是开发了一种新方法来自洽地描述具有异质耦合的复合体中的能量传递。采用实验确定的光谱密度来计算能量转移率。合理地再现了配合物在室温下的吸收光谱和荧光衰减时间成分。讨论了特殊叶绿素分子（分别为红色分子、连接分子和反应中心分子）的作用。捕获时间的正式精确表达式是根据固有捕获时间、捕获的平均首次通过时间和去捕获时间得出的。讨论了能量转移机制，发现到达初级电子供体的最慢步骤包含两个主要步骤：转移到反应中心和从反应中心转移到陷阱。本征电荷转移时间估计为0.8∼1.7ps。讨论了计算的跃迁能量的捕获时间和 Chls 方向的最优性。
We model the energy transfer and trapping kinetics in PSI. Rather than simply applying Förster theory, we develop a new approach to self-consistently describe energy transfer in a complex with heterogeneous couplings. Experimentally determined spectral densities are employed to calculate the energy transfer rates. The absorption spectrum and fluorescence decay time components of the complex at room temperature were reasonably reproduced. The roles of the special chlorophylls (red, linker, and reaction center, respectively) molecules are discussed. A formally exact expression for the trapping time is derived in terms of the intrinsic trapping time, mean first passage time to trap, and detrapping time. The energy transfer mechanism is discussed and the slowest steps of the arrival at the primary electron donor are found to contain two dominant steps:transfer-to-reaction-center, andtransfer-to-trap-from-reaction-center. The intrinsic charge transfer time is estimated to be 0.8∼1.7ps. The optimality with respect to the trapping time of the calculated transition energies and the orientation of Chls is discussed.
K.Mitsuke；T.Kondow；K.Kuchitsu：J.里斯。
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