Unrestricted density functional theory based on the fragment molecular orbital method for the ground and excited state calculations of large systems

作者：Nakata Hiroya^*; Fedorov Dmitri G; Yokojima Satoshi; Kitaura Kazuo; Sakurai Minoru; Nakamura Shinichiro

来源：Journal of Chemical Physics, 2014, 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.

• 出版日期2014-4-14
• 单位RIKEN