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Title: Development of reactive force fields using ab initio molecular dynamics simulation minimally biased to experimental data

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.4985903· OSTI ID:1512315
 [1];  [2]; ORCiD logo [2]
  1. Univ. of Chicago, IL (United States). Dept. of Chemistry. James Franck Inst. Inst. for Biophysical Dynamics; Wuhan Univ. (China). College of Chemistry and Molecular Sciences. Hubei Key Lab. of Electrochemical Power Sources
  2. Univ. of Chicago, IL (United States). Dept. of Chemistry. James Franck Inst. Inst. for Biophysical Dynamics
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Incorporation of quantum mechanical electronic structure data is necessary to properly capture the physics of many chemical processes. Proton hopping in water, which involves rearrangement of chemical and hydrogen bonds, is one such example of an inherently quantum mechanical process. Standard ab initio molecular dynamics (AIMD) methods, however, do not yet accurately predict the structure of water and are therefore less than optimal for developing force fields. We have instead utilized a recently developed method which minimally biases AIMD simulations to match limited experimental data to develop novel multiscale reactive molecular dynamics (MS-RMD) force fields by using relative entropy minimization. In this paper, we present two new MS-RMD models using such a parameterization: one which employs water with harmonic internal vibrations and another which uses anharmonic water. We show that the newly developed MS-RMD models very closely reproduce the solvation structure of the hydrated excess proton in the target AIMD data. We also find that the use of anharmonic water increases proton hopping, thereby increasing the proton diffusion constant.

Research Organization:
Univ. of Chicago, IL (United States); Wuhan Univ. (China)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Natural Science Foundation of China (NSFC); China Scholarship Council
Grant/Contract Number:
SC0005418; 21303123; 21303124; 201306275019
OSTI ID:
1512315
Alternate ID(s):
OSTI ID: 1373443; OSTI ID: 1582246
Journal Information:
Journal of Chemical Physics, Vol. 147, Issue 16; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 12 works
Citation information provided by
Web of Science

References (35)

Defining Condensed Phase Reactive Force Fields from ab Initio Molecular Dynamics Simulations: The Case of the Hydrated Excess Proton journal September 2010
The quest for the best nonpolarizable water model from the adaptive force matching method journal August 2010
A Direct Method for Incorporating Experimental Data into Multiscale Coarse-Grained Models journal April 2016
Relative entropy as a universal metric for multiscale errors journal June 2010
A second generation multistate empirical valence bond model for proton transport in aqueous systems journal September 2002
Ab initio molecular dynamics simulation of the solvation and transport of hydronium and hydroxyl ions in water journal July 1995
The quantum dynamics of an excess proton in water journal February 1996
A Refined MS-EVB Model for Proton Transport in Aqueous Environments journal December 2011
Ab initio molecular dynamics of liquid water using embedded-fragment second-order many-body perturbation theory towards its accurate property prediction journal September 2015
Development of a “First Principles” Water Potential with Flexible Monomers: Dimer Potential Energy Surface, VRT Spectrum, and Second Virial Coefficient journal November 2013
Anomalous waterlike behavior in spherically-symmetric water models optimized with the relative entropy journal January 2009
An Improved Multistate Empirical Valence Bond Model for Aqueous Proton Solvation and Transport † journal January 2008
The nature of the hydrated excess proton in water journal February 1999
An analysis of hydrated proton diffusion in ab initio molecular dynamics journal January 2015
Comparison of simple potential functions for simulating liquid water journal July 1983
Communication: Improved ab initio molecular dynamics by minimally biasing with experimental data journal January 2017
Predicting the melting temperature of ice-Ih with only electronic structure information as input journal July 2012
A general purpose model for the condensed phases of water: TIP4P/2005 journal December 2005
Efficient and Minimal Method to Bias Molecular Simulations with Experimental Data journal July 2014
Accurate description of van der Waals complexes by density functional theory including empirical corrections journal January 2004
The relative entropy is fundamental to multiscale and inverse thermodynamic problems journal October 2008
The computer simulation of proton transport in water journal November 1999
Reactive molecular dynamics models from ab initio molecular dynamics data using relative entropy minimization journal September 2017
Coarse-graining errors and numerical optimization using a relative entropy framework journal March 2011
Flexible simple point-charge water model with improved liquid-state properties journal January 2006
Modeling Molecular Interactions in Water: From Pairwise to Many-Body Potential Energy Functions journal May 2016
Development of a “First-Principles” Water Potential with Flexible Monomers. III. Liquid Phase Properties journal July 2014
The missing term in effective pair potentials journal November 1987
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu journal April 2010
Effects of the dispersion interaction in liquid water journal September 2011
Approaching post-Hartree–Fock quality potential energy surfaces with simple pair-wise expressions: parameterising point-charge-based force fields for liquid water using the adaptive force matching method journal June 2011
Role of Presolvation and Anharmonicity in Aqueous Phase Hydrated Proton Solvation and Transport journal November 2015
The Curious Case of the Hydrated Proton journal August 2011
Perspective: How good is DFT for water? journal April 2016
Multiscale reactive molecular dynamics journal December 2012

Cited By (3)

Recent advances in quantum‐mechanical molecular dynamics simulations of proton transfer mechanism in various water‐based environments journal May 2019
Correlated dynamics in aqueous proton diffusion journal January 2018
Correlated Dynamics in Aqueous Proton Diffusion text January 2018

Figures / Tables (4)

FIG. 1(p. 5)figure FIG. 1
FIG. 2(p. 6)figure FIG. 2
FIG. 3(p. 7)figure FIG. 3
FIG. 4(p. 7)figure FIG. 4

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Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
reactive force field
chemical elements
hydrogen bonding
water model
molecular dynamics
mass diffusion
entropy
ions and properties
quantum effects
chemical processes