Petrov Elmar G, Robert Bruno, Lin Sheng Hsien, Valkunas Leonas
Bogolyubov Institute for Theoretical Physics, National Academy of Sciences of Ukraine, Kiev, Ukraine.
Nuclear Research Center Saclay, UMR 8221 Centre National de la Recherche Scientifique, Institut de Biologie et de Technologie de Saclay, University Paris Sud, Gif sur Yvette, France.
Biophys J. 2015 Oct 20;109(8):1735-45. doi: 10.1016/j.bpj.2015.08.026.
Theoretical consideration is presented of the triplet excitation dynamics in donor-acceptor systems in conditions where the transfer is mediated by an oxygen molecule. It is demonstrated that oxygen may be involved in both real and virtual intramolecular triplet-singlet conversions in the course of the process under consideration. Expressions describing a superexchange donor-acceptor coupling owing to a participation of the bridging twofold degenerate oxygen's virtual singlet state are derived and the transfer kinetics including the sequential (hopping) and coherent (distant) routes are analyzed. Applicability of this theoretical description to the pigment-protein complex cytochrome b6f, by considering the triplet excitation transfer from the chlorophyll a molecule to distant β-carotene, is discussed.
本文给出了在氧分子介导转移的条件下,供体-受体系统中三重态激发动力学的理论考量。结果表明,在所考虑的过程中,氧可能参与了真实的和虚拟的分子内三重态-单重态转换。推导了描述由于桥连的双重简并氧的虚拟单重态参与而产生的超交换供体-受体耦合的表达式,并分析了包括顺序(跳跃)和相干(远程)途径的转移动力学。通过考虑从叶绿素a分子到远距离β-胡萝卜素的三重态激发转移,讨论了该理论描述对色素-蛋白质复合物细胞色素b6f的适用性。