Nakata Hiroya, Fedorov Dmitri G, Yokojima Satoshi, Kitaura Kazuo, Sakurai Minoru, Nakamura Shinichiro
Center for Biological Resources and Informatics, Tokyo Institute of Technology, B-62 4259 Nagatsuta-cho, Midori-ku, Yokohama 226-8501, Japan.
NRI, National Institute of Advanced Industrial Science and Technology (AIST), 1-1-1 Umezono, Tsukuba, Ibaraki 305-8568, Japan.
J Chem Phys. 2014 Apr 14;140(14):144101. doi: 10.1063/1.4870261.
We extended the fragment molecular orbital (FMO) method interfaced with density functional theory (DFT) into spin unrestricted formalism (UDFT) and developed energy gradients for the ground state and single point excited state energies based on time-dependent DFT. The accuracy of FMO is evaluated in comparison to the full calculations without fragmentation. Electronic excitations in solvated organic radicals and in the blue copper protein, plastocyanin (PDB code: 1BXV), are reported. The contributions of solvent molecules to the electronic excitations are analyzed in terms of the fragment polarization and quantum effects such as interfragment charge transfer.
我们将与密度泛函理论（DFT）相结合的片段分子轨道（FMO）方法扩展到自旋非限制形式（UDFT），并基于含时密度泛函理论开发了基态和单点激发态能量的能量梯度。通过与无片段的全计算进行比较，评估了FMO的准确性。报告了溶剂化有机自由基和蓝铜蛋白质体蓝素（PDB代码：1BXV）中的电子激发。从片段极化和量子效应（如片段间电荷转移）的角度分析了溶剂分子对电子激发的贡献。
