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In photosynthesis, pigment-excitation energies in the antenna system produced by light harvesting are transferred among antenna pigments toward the core antenna, where they are captured by the reaction center and initially fixed in the form of a charge separation. Primary charge separation between an oxidized special pair (P+) and a reduced bacteriopheohytin (H−) is occasionally intervened by recombination, and a spin-triplet state (3P*) is formed on P in the bacterial reaction center. The 3P* state is harmful to bio-organisms, inducing the formation of the highly damaging singlet oxygen species. Therefore, understanding the 3P*-formation mechanism is important. The 3P* formation is mediated by a state |m〉 of intermediate charge separation between P and the accessory chlorophyll, which is located between P and H. It will be shown theoretically in the present work that at room temperature, not only the mechanism of superexchange by quantum-mechanical virtual mediation at |m〉, but also a hot-sequential mechanism contributes to the mediation. In the latter, although |m〉 is produced as a real state, the final state 3P* is quickly formed during thermalization of phonons in the protein matrix in |m〉. In the former, the final state is formed more quickly before dephasing-thermalization of phonons in |m〉. 3P* is unistep formed from the charge-separated state in the both mechanisms. 相似文献
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