title: Importance of Three-Body Interactions in Molecular Dynamics Simulations of Water Demonstrated with the Fragment Molecular Orbital Method.
abstract: The analytic first derivative with respect to nuclear coordinates is formulated and implemented in the framework of the three-body fragment molecular orbital (FMO) method. The gradient has been derived and implemented for restricted second-order Møller-Plesset perturbation theory, as well as for both restricted and unrestricted Hartree-Fock and density functional theory. The importance of the three-body fully analytic gradient is illustrated through the failure of the two-body FMO method during molecular dynamics simulations of a small water cluster. The parallel implementation of the fragment molecular orbital method, its parallel efficiency, and its scalability on the Blue Gene/Q architecture up to 262,144 CPU cores are also discussed.
authors.affiliation: Argonne Leadership Computing Facility, Argonne National Laboratory , 9700 S. Cass Avenue, Lemont, Illinois 60439, United States.
authors.forename: Spencer R
authors.initials: SR
authors.lastname: Pruitt
authors.affiliation: Department of Fundamental Technology Research, R&D Center Kagoshima, Kyocera Corporation , 1-4 Kokubu Yamashita-cho, Kirishima-shi, Kagoshima 899-4312, Japan.
authors.forename: Hiroya
authors.initials: H
authors.lastname: Nakata
authors.affiliation: Nanosystem Research Institute, National Institute of Advanced Industrial Science and Technology , 1-1-1 Umenzono, Tsukuba, Ibaraki 305-8568, Japan.
authors.forename: Takeshi
authors.initials: T
authors.lastname: Nagata
authors.affiliation: Department of Chemistry and Biochemistry, University of Massachusetts Dartmouth , 285 Old Westport Road, Dartmouth, Massachusetts 02747-2300, United States.
authors.forename: Maricris
authors.initials: M
authors.lastname: Mayes
authors.affiliation: Argonne Leadership Computing Facility, Argonne National Laboratory , 9700 S. Cass Avenue, Lemont, Illinois 60439, United States.
authors.forename: Yuri
authors.initials: Y
authors.lastname: Alexeev
authors.affiliation: Argonne Leadership Computing Facility, Argonne National Laboratory , 9700 S. Cass Avenue, Lemont, Illinois 60439, United States.
authors.forename: Graham
authors.initials: G
authors.lastname: Fletcher
authors.affiliation: Nanosystem Research Institute, National Institute of Advanced Industrial Science and Technology , 1-1-1 Umenzono, Tsukuba, Ibaraki 305-8568, Japan.
authors.forename: Dmitri G
authors.initials: DG
authors.lastname: Fedorov
authors.affiliation: Graduate School of System Informatics, Kobe University , 1-1 Rokkodai-cho, Nada-ku, Kobe 657-8501, Japan.
authors.forename: Kazuo
authors.initials: K
authors.lastname: Kitaura
authors.affiliation: Department of Chemistry and Ames Laboratory, Iowa State University , 201 Spedding Hall, Ames, Iowa 50011, United States.
authors.forename: Mark S
authors.initials: MS
authors.lastname: Gordon