Development of QM/MM hybrid method for strongly correlated systems and its applications to reaction centers of bioenzyemes

2011年，介绍了光系统II的水氧化反应中心的结构。我们利用它们的X射线结构进行了计算，并公布了它们结构的电子和自旋结构的结果，其中我们研究了所有可能的氧化态和所有可能的自旋结构。据我们所知，这是第一篇关于光系统II的Mn团簇的计算结果的论文。随后，我们研究了自然轨道和几何变化，提出了氧化水分子的可能反应机理。另一方面，由于计算结果与实验结果之间略有矛盾，我们通过构建原始的锰配合物测试集，考察了锰配合物磁性描述的函数依赖性。我们还研究了Mn团簇的非共线磁性，提出了基于自旋密度线性响应函数的QM/MM边界准则。

In 2011, the structure of the the water oxydation reaction center of photosystem II is presented. We performed calculations with using their X-ray structure and published the results of electronic ans spin structures of their structure, in which we examined all possible oxidation states with all possible spin structures. To our knowledge, this is the first paper on computational results of the Mn clusters of photosystem II. Subsequently, we examined natural orbitals and geometry changes to propose the possible reaction mechanisms to oxidize the water molecules. On the other side, because there is slight contradiction between calculational results and experimental results, we examined functional dependency of the description of magnetism of Mn complexes with constructing original test sets of Mn complexes. We also examined noncollinear magnetism of Mn clusters and proposed a QM/MM boundary guideline based on linear response function of spin density.