title: Ab Initio Extension of the AMOEBA Polarizable Force Field to Fe(2.).
abstract: We extend the AMOEBA polarizable molecular mechanics force field to the Fe(2+) cation in its singlet, triplet, and quintet spin states. Required parameters are obtained either directly from first principles calculations or optimized so as to reproduce corresponding interaction energy components in a hexaaquo environment derived from quantum mechanical energy decomposition analyses. We assess the importance of the damping of point-dipole polarization at short distance as well as the influence of charge-transfer for metal-water interactions in hydrated Fe(2+); this analysis informs the selection of model systems employed for parametrization. We validate our final Fe(2+) model through comparison of molecular dynamics (MD) simulations to available experimental data for aqueous ferrous ion in its quintet electronic ground state.
authors.affiliation: Department of Chemistry, Chemical Theory Center, and Supercomputing Institute, University of Minnesota , 207 Pleasant St. SE, Minneapolis, Minnesota 55455, United States.
authors.forename: David
authors.initials: D
authors.lastname: Semrouni
authors.affiliation: Department of Chemistry, Chemical Theory Center, and Supercomputing Institute, University of Minnesota , 207 Pleasant St. SE, Minneapolis, Minnesota 55455, United States.
authors.forename: William C
authors.initials: WC
authors.lastname: Isley
authors.affiliation: Laboratoire des Mécanismes Réactionnels, Département de Chimie, École Polytechnique, CNRS , 91128 Palaiseau Cedex, France.
authors.forename: Carine
authors.initials: C
authors.lastname: Clavaguéra
authors.affiliation: CEA/Saclay , UMR 3299 CEA/CNRS SIS2M, Laboratoire de Chimie de Coordination des Eléments f, F-91191 Gif-sur-Yvette, France.
authors.forename: Jean-Pierre
authors.initials: JP
authors.lastname: Dognon
authors.affiliation: Department of Chemistry, Chemical Theory Center, and Supercomputing Institute, University of Minnesota , 207 Pleasant St. SE, Minneapolis, Minnesota 55455, United States.
authors.forename: Christopher J
authors.initials: CJ
authors.lastname: Cramer
authors.affiliation: Department of Chemistry, Chemical Theory Center, and Supercomputing Institute, University of Minnesota , 207 Pleasant St. SE, Minneapolis, Minnesota 55455, United States.
authors.forename: Laura
authors.initials: L
authors.lastname: Gagliardi