Energy-transfer and charge-separation pathways in the reaction center of photosystem II revealed by coherent two-dimensional optical spectroscopy
Energy-transfer and charge-separation pathways in the reaction center of photosystem II revealed by coherent two-dimensional optical spectroscopy
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DOI：
10.1063/1.3493580
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发表时间：
2010-11-14
影响因子：
4.4
通讯作者：
Mukamel, Shaul
中科院分区：
文献类型：
--
作者：
Abramavicius, Darius;Mukamel, Shaul
用双带紧束缚模型模拟了光系统II光合作用反应中心电子和空穴的激发态动力学和驰豫过程。用输运理论计算了耗散激子和载流子运动，该理论包含了与具有实验确定的谱密度的谐波浴的强耦合，并在适当的参数范围内简化为Redfield、Forster和Marcus表达式。在-k(1)+k(2)+k(3)、k(1)-k(2)+k(3)和k(1)+k(2)-k(3)方向产生的三阶二维信号清楚地揭示了激子迁移和电荷分离过程。(C)2010年美国物理研究所。[DOI：10.1063/1.3493580]
The excited state dynamics and relaxation of electrons and holes in the photosynthetic reaction center of photosystem II are simulated using a two-band tight-binding model. The dissipative exciton and charge carrier motions are calculated using a transport theory, which includes a strong coupling to a harmonic bath with experimentally determined spectral density, and reduces to the Redfield, the Forster, and the Marcus expressions in the proper parameter regimes. The simulated third order two-dimensional signals, generated in the directions -k(1)+k(2)+k(3), k(1)-k(2)+k(3), and k(1)+k(2)-k(3), clearly reveal the exciton migration and the charge-separation processes. (C) 2010 American Institute of Physics. [doi:10.1063/1.3493580]