title: Development and validation of a ReaxFF reactive force field for Cu cation/water interactions and copper metal/metal oxide/metal hydroxide condensed phases.
abstract: To enable large-scale reactive dynamic simulations of copper oxide/water and copper ion/water interactions we have extended the ReaxFF reactive force field framework to Cu/O/H interactions. To this end, we employed a multistage force field development strategy, where the initial training set (containing metal/metal oxide/metal hydroxide condensed phase data and [Cu(H(2)O)(n)](2+) cluster structures and energies) is augmented by single-point quantum mechanices (QM) energies from [Cu(H(2)O)(n)](2+) clusters abstracted from a ReaxFF molecular dynamics simulation. This provides a convenient strategy to both enrich the training set and to validate the final force field. To further validate the force field description we performed molecular dynamics simulations on Cu(2+)/water systems. We found good agreement between our results and earlier experimental and QM-based molecular dynamics work for the average Cu/water coordination, Jahn-Teller distortion, and inversion in [Cu(H(2)O)(6)](2+) clusters and first- and second-shell O-Cu-O angular distributions, indicating that this force field gives a satisfactory description of the Cu-cation/water interactions. We believe that this force field provides a computationally convenient method for studying the solution and surface chemistry of metal cations and metal oxides and, as such, has applications for studying protein/metal cation complexes, pH-dependent crystal growth/dissolution, and surface catalysis.
authors: Department of Mechanical and Nuclear Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, USA. acv13@psu.edu
authors: Adri C T
authors: AC
authors: van Duin
authors: Vyacheslav S
authors: VS
authors: Bryantsev
authors: Mamadou S
authors: MS
authors: Diallo
authors: William A
authors: WA
authors: Goddard
authors: Obaidur
authors: O
authors: Rahaman
authors: Douglas J
authors: DJ
authors: Doren
authors: David
authors: D
authors: Raymand
authors: Kersti
authors: K
authors: Hermansson
mesh_terms: D003300:Copper / Q000737:chemistry*; D006863:Hydrogen-Ion Concentration; D006878:Hydroxides / Q000737:chemistry*; D056004:Molecular Dynamics Simulation; D011789:Quantum Theory; D013499:Surface Properties; D014867:Water / Q000737:chemistry*
chemical_list: D006878:Hydroxides; C508959:copper hydroxide; D014867:Water; D003300:Copper; C030973:cupric oxide