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Derivatives of the approximated electrostatic potentials in unrestricted Hartree–Fock based on the fragment molecular orbital method and an application to polymer radicals

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Abstract

The analytic energy gradient for the point charge approximation of the embedding potential is derived in the framework of unrestricted Hartree–Fock based on the fragment molecular orbital method (FMO). For this goal, we derive the necessary coupled-perturbed unrestricted Hartree–Fock equations, describing the response terms arising from the use of embedding atomic charges in dimer calculations. By a comparison to numerical gradients and with the aid of molecular dynamics, we show that the gradients have a high accuracy. A speed-up of the factor 7.3 is obtained for the largest system, when approximated potentials are used relative to the exact two-electron embedding. We apply the FMO method to polymer radicals and show that it has satisfactory accuracy in reproducing the geometries and energies of polymer radical reactions.

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Acknowledgments

We thank late Dr. Takeshi Nagata for helpful discussions about the FMO analytic energy gradient. This work was in part supported by the Next Generation Super Computing Project, Nanoscience Program (MEXT, Japan) and Computational Materials Science Initiative (CMSI, Japan). Most calculations were performed on TSUBAME2.0 at the Global Scientific Information and Computing Center of Tokyo Institute of Technology. We also thank the RIKEN Integrated Cluster of Clusters (RICC) at RIKEN and Research Center for Computational Science (Okazaki, Japan) for the computer resources.

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Authors and Affiliations

  1. Department of Biomolecular Engineering, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, Kanagawa, 226-8501, Japan

    Hiroya Nakata

  2. Research Cluster for Innovation, Nakamura Lab, 2-1 Hirosawa, Wako, Saitama, 351-0198, Japan

    Hiroya Nakata, Satoshi Yokojima & Shinichiro Nakamura

  3. NRI, National Institute of Advanced Industrial Science and Technology (AIST), 1-1-1 Umezono, Tsukuba, Ibaraki, 305-8568, Japan

    Dmitri G. Fedorov

  4. Tokyo University of Pharmacy and Life Sciences, 1423-1 Horinouchi, Hachiouji-shi, Tokyo, 192-0392, Japan

    Satoshi Yokojima

  5. Graduate School of System Informatics, Kobe University, 1-1 Rokkodai-cho, Nada-ku, Kobe, 657-8501, Japan

    Kazuo Kitaura

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  1. Hiroya Nakata
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  2. Dmitri G. Fedorov
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  3. Satoshi Yokojima
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  4. Kazuo Kitaura
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  5. Shinichiro Nakamura
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Correspondence to Hiroya Nakata.

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Nakata, H., Fedorov, D.G., Yokojima, S. et al. Derivatives of the approximated electrostatic potentials in unrestricted Hartree–Fock based on the fragment molecular orbital method and an application to polymer radicals. Theor Chem Acc 133, 1477 (2014). https://doi.org/10.1007/s00214-014-1477-6

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