Mechanism and Unidirectionality of the Electron Transfer in the Photosynthetic Reaction Center of Rhodopseudomonas Viridis: SAC−CI Theoretical Study
Mechanism and Unidirectionality of the Electron Transfer in the Photosynthetic Reaction Center of Rhodopseudomonas Viridis: SAC−CI Theoretical Study
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绿色红假单胞菌光合反应中心电子传递机制及单向性：SAC−CI 理论研究
DOI：
10.1021/jp982870x
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发表时间：
1998
影响因子：
3.3
通讯作者：
H. Nakatsuji
中科院分区：
文献类型：
--
作者：
J. Hasegawa;H. Nakatsuji
采用对称适应簇(SAC) -组态相互作用（CI）方法，从理论上研究了绿Rhodopseudomonas （Rps）光合反应中心（PSRC）光激发特殊对电子向细菌叶绿素单向性转移的电子机制和原因。利用点电荷模型考虑了周围蛋白质的影响。电子转移的l支选择性可以用转移积分的不对称性来解释，这是一个电子因子，它源于PSRC的一个小的结构不对称性：l侧的发色团在局部比m侧的发色团更接近，尽管平均分离几乎相同。电荷复合速率的小是由于特殊对LUMO和HOMO之间的电子定位不同。在静电模型有效的范围内，蛋白质对单向性的影响是很小的，尽管蛋白质保持了三维定向。
The electronic mechanism and the origin of the unidirectionality of the electron transfer from photoexcited special pair to bacteriopheophytin in the photosynthetic reaction center (PSRC) of Rhodopseudomonas (Rps) viridis are studied theoretically by using the SAC(symmetry adapted cluster)−CI (configuration interaction) method. The effects of the surrounding proteins are considered by using the point charge model. The L-branch selectivity of the electron transfer is explained by the asymmetry of the transfer integral, an electronic factor, which originates from a small structural asymmetry of the PSRC: the L-side chromophores are locally closer than the M-side ones, though the average separations are almost the same. The smallness of the charge recombination rate is attributed to the difference in the electron localization between the LUMO and HOMO of special pair. Protein effects on the unidirectionality are quite small as far as the electrostatic model is valid, though the proteins keep the three-dimen...