A new computational scheme to analyze electron transfer (ET) pathways in large biomolecules is presented with applications to ETs in bacterial photosynthetic reaction center. It consists of a linear combination of fragment molecular orbitals and an electron tunneling current analysis, which enables an efficient first-principles analysis of ET pathways in large biomolecules. The scheme has been applied to the ET from menaquinone to ubiquinone via nonheme iron complex in bacterial photosynthetic reaction center. It has revealed that not only the central Fe$^{2+}$ ion but also particular histidine ligands are involved in the ET pathways in such a way to mitigate perturbations that can be caused by metal ion substitution and depletion, which elucidates the experimentally observed insensitivity of the ET rate to these perturbations.
Vibronic Landscape of Excitons in Photosynthetic Antenna
Institute of Integrative Biology of the Cell, CEA, CNRS, Université Paris Saclay（细胞整合生物学研究所）；Laboratoire d’ingénierie des systèmes moléculaires, CNRS, Aix-Marseille University（分子系统工程实验室）；Department of Molecular Compound Physics, Centre for Physical Sciences and Technology（物理化学中心）
Efficiency of energy funneling in the photosystem II supercomplex of higher plants
光合多蛋白质网络中能量传递特性的研究有助于深入了解其设计原理。本文讨论了高等植物光合机构中最大的功能单元--光系统II（PS-II）C $_2$ S $_2$ M $_2$超复合体的激子能量传递机制。尽管C $_2$ S $_2$ M $_2$中缺乏决定性的能量梯度，我们表明，能量转移是由弛豫指向低能态。C $_2$ S $_2$ M $_2$没有被组织成形成具有严格的能量向下转移的途径，这对转移效率、转移途径和转移限制步骤具有直接的后果。激子动力学对小的结构变化很敏感，例如，由振动坐标的重组引起的结构变化。为了将重组过程中，我们的数值模拟，我们超越速率方程，并使用分层耦合运动方程的方法（HEOM）。虽然从外周天线到反应中心附近的蛋白质的转移发生在更快的时间尺度上，但能量转移到RC核心的最后一步相当慢，因此是转移链中的限制步骤。我们的研究结果表明，PS-II超复合物的结构保证光保护，而不是优化效率。
Modular molecular toolkit for photochemical energy conversion in a self-assembling nanocontainer
University of South Bohemia（南波希米亚大学）；Czech Academy of Sciences, Institute of Microbiology, Centre Algatech（捷克科学院微生物学研究所阿尔加技术中心）；Czech Academy of Sciences, Biology Centre, Institute of Plant Molecular Biology（捷克科学院生物中心植物分子生物学研究所）；Charles University, Faculty of Science, Department of Analytical Chemistry（查理大学理学院分析化学系）；Charles University, Faculty of Mathematics and Physics, Department of Chemical Physics and Optics（查理大学数学与物理学院化学物理与光学系）；The University of British Columbia, Department of Microbiology & Immunology（不列颠哥伦比亚大学生物学与免疫学系）
