Keywords

Water model, Molecular dynamics, Reactive force field, Transport properties, Electrostatics, Central-force, Polarizability, Computer simulation, Interatomic potentials, Classical statistical mechanics

Abstract

A new polarizable water model is developed for molecular dynamics (MD) simulations of the proton transport process. The interatomic potential model has three important submodels corresponding to electrostatic interactions, making and breaking of covalent bonds, and treatment of electron exchange and correlation through a van der Waals potential. A polarizable diffuse charge density function was used to describe Coulombic interactions between atoms. Most of the model parameters were obtained from ab initio data for a lone water molecule. Molecules respond realistically to their electrochemical environment by the use of coupled fluctuating charge and fluctuating dipole dynamics, which controlled the charge density. The main purpose of the work is to develop a general model and framework for future studies, though some validation work was performed here. We applied the model to a MD simulation study of bulk properties of liquid water at room temperature and model gave good agreement with thermodynamic and transport properties at the same conditions. The model was then applied to a preliminary study of proton transfer, in which multiple proton transfer events were observed, though the rate of proton transfer was under-predicted by a factor of 5.

Original Publication Citation

Abhishek Asthana, Dean R. Wheeler; A polarizable reactive force field for water to enable molecular dynamics simulations of proton transport. J. Chem. Phys. 7 May 2013; 138 (17): 174502. https://doi.org/10.1063/1.4798457

Document Type

Peer-Reviewed Article

Publication Date

2013-05-07

Publisher

American Institute of Physics

Language

English

College

Ira A. Fulton College of Engineering

Department

Chemical Engineering

University Standing at Time of Publication

Full Professor

Download

Share

COinS