Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

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

Abstract

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.

Authors:
 [1];  [2]; ORCiD logo [2]
+ Show Author Affiliations
  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
Publication Date:
Research Org.:
Univ. of Chicago, IL (United States); Wuhan Univ. (China)
Sponsoring Org.:
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
OSTI Identifier:
1512315
Alternate Identifier(s):
OSTI ID: 1373443; OSTI ID: 1582246
Grant/Contract Number:  
SC0005418; 21303123; 21303124; 201306275019
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 147; Journal Issue: 16; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
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

Citation Formats

Chen, Chen, Arntsen, Christopher, and Voth, Gregory A. Development of reactive force fields using ab initio molecular dynamics simulation minimally biased to experimental data. United States: N. p., 2017. Web. doi:10.1063/1.4985903.
Copy to clipboard
Chen, Chen, Arntsen, Christopher, & Voth, Gregory A. Development of reactive force fields using ab initio molecular dynamics simulation minimally biased to experimental data. United States. https://doi.org/10.1063/1.4985903
Copy to clipboard
Chen, Chen, Arntsen, Christopher, and Voth, Gregory A. Tue . "Development of reactive force fields using ab initio molecular dynamics simulation minimally biased to experimental data". United States. https://doi.org/10.1063/1.4985903. https://www.osti.gov/servlets/purl/1512315.
Copy to clipboard
@article{osti_1512315,
title = {Development of reactive force fields using ab initio molecular dynamics simulation minimally biased to experimental data},
author = {Chen, Chen and Arntsen, Christopher and Voth, Gregory A.},
abstractNote = {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.},
doi = {10.1063/1.4985903},
journal = {Journal of Chemical Physics},
number = 16,
volume = 147,
place = {United States},
year = {Tue Aug 01 00:00:00 EDT 2017},
month = {Tue Aug 01 00:00:00 EDT 2017}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1063/1.4985903
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 12 works
Citation information provided by
Web of Science

Figures / Tables:

FIG. 1 FIG. 1: Radial distribution functions for AIMD, EDS-AIMD, MS-RMD 4, and MS-RMD 5. The oxygen and hydrogen atoms denoted with an asterisk are for hydronium oxygen and hydrogen nuclei. The subscript “w” denotes a water molecule.
All figures and tables (4 total)
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Defining Condensed Phase Reactive Force Fields from ab Initio Molecular Dynamics Simulations: The Case of the Hydrated Excess Proton
journal, September 2010

  • Knight, Chris; Maupin, C. Mark; Izvekov, Sergei
  • Journal of Chemical Theory and Computation, Vol. 6, Issue 10
  • DOI: 10.1021/ct1004438

The quest for the best nonpolarizable water model from the adaptive force matching method
journal, August 2010

  • Akin-Ojo, Omololu; Wang, Feng
  • Journal of Computational Chemistry, Vol. 32, Issue 3
  • DOI: 10.1002/jcc.21634

A Direct Method for Incorporating Experimental Data into Multiscale Coarse-Grained Models
journal, April 2016

  • Dannenhoffer-Lafage, Thomas; White, Andrew D.; Voth, Gregory A.
  • Journal of Chemical Theory and Computation, Vol. 12, Issue 5
  • DOI: 10.1021/acs.jctc.6b00043

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

  • Day, Tyler J. F.; Soudackov, Alexander V.; Čuma, Martin
  • The Journal of Chemical Physics, Vol. 117, Issue 12
  • DOI: 10.1063/1.1497157

Ab initio molecular dynamics simulation of the solvation and transport of hydronium and hydroxyl ions in water
journal, July 1995

  • Tuckerman, M.; Laasonen, K.; Sprik, M.
  • The Journal of Chemical Physics, Vol. 103, Issue 1
  • DOI: 10.1063/1.469654

The quantum dynamics of an excess proton in water
journal, February 1996

  • Lobaugh, J.; Voth, Gregory A.
  • The Journal of Chemical Physics, Vol. 104, Issue 5
  • DOI: 10.1063/1.470962

A Refined MS-EVB Model for Proton Transport in Aqueous Environments
journal, December 2011

  • Park, Kyoyeon; Lin, Wei; Paesani, Francesco
  • The Journal of Physical Chemistry B, Vol. 116, Issue 1
  • DOI: 10.1021/jp208946p

Ab initio molecular dynamics of liquid water using embedded-fragment second-order many-body perturbation theory towards its accurate property prediction
journal, September 2015

  • Willow, Soohaeng Yoo; Salim, Michael A.; Kim, Kwang S.
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep14358

Development of a “First Principles” Water Potential with Flexible Monomers: Dimer Potential Energy Surface, VRT Spectrum, and Second Virial Coefficient
journal, November 2013

  • Babin, Volodymyr; Leforestier, Claude; Paesani, Francesco
  • Journal of Chemical Theory and Computation, Vol. 9, Issue 12
  • DOI: 10.1021/ct400863t

Anomalous waterlike behavior in spherically-symmetric water models optimized with the relative entropy
journal, January 2009

  • Chaimovich, Aviel; Shell, M. Scott
  • Physical Chemistry Chemical Physics, Vol. 11, Issue 12
  • DOI: 10.1039/b818512c

An Improved Multistate Empirical Valence Bond Model for Aqueous Proton Solvation and Transport †
journal, January 2008

  • Wu, Yujie; Chen, Hanning; Wang, Feng
  • The Journal of Physical Chemistry B, Vol. 112, Issue 2
  • DOI: 10.1021/jp076658h

The nature of the hydrated excess proton in water
journal, February 1999

  • Marx, Dominik; Tuckerman, Mark E.; Hutter, Jürg
  • Nature, Vol. 397, Issue 6720
  • DOI: 10.1038/17579

An analysis of hydrated proton diffusion in ab initio molecular dynamics
journal, January 2015

  • Tse, Ying-Lung Steve; Knight, Chris; Voth, Gregory A.
  • The Journal of Chemical Physics, Vol. 142, Issue 1
  • DOI: 10.1063/1.4905077

Comparison of simple potential functions for simulating liquid water
journal, July 1983

  • Jorgensen, William L.; Chandrasekhar, Jayaraman; Madura, Jeffry D.
  • The Journal of Chemical Physics, Vol. 79, Issue 2
  • DOI: 10.1063/1.445869

Communication: Improved ab initio molecular dynamics by minimally biasing with experimental data
journal, January 2017

  • White, Andrew D.; Knight, Chris; Hocky, Glen M.
  • The Journal of Chemical Physics, Vol. 146, Issue 4
  • DOI: 10.1063/1.4974837

Predicting the melting temperature of ice-Ih with only electronic structure information as input
journal, July 2012

  • Pinnick, Eric R.; Erramilli, Shyamsunder; Wang, Feng
  • The Journal of Chemical Physics, Vol. 137, Issue 1
  • DOI: 10.1063/1.4731693

A general purpose model for the condensed phases of water: TIP4P/2005
journal, December 2005

  • Abascal, J. L. F.; Vega, C.
  • The Journal of Chemical Physics, Vol. 123, Issue 23
  • DOI: 10.1063/1.2121687

Efficient and Minimal Method to Bias Molecular Simulations with Experimental Data
journal, July 2014

  • White, Andrew D.; Voth, Gregory A.
  • Journal of Chemical Theory and Computation, Vol. 10, Issue 8
  • DOI: 10.1021/ct500320c

Accurate description of van der Waals complexes by density functional theory including empirical corrections
journal, January 2004

  • Grimme, Stefan
  • Journal of Computational Chemistry, Vol. 25, Issue 12
  • DOI: 10.1002/jcc.20078

The relative entropy is fundamental to multiscale and inverse thermodynamic problems
journal, October 2008

  • Shell, M. Scott
  • The Journal of Chemical Physics, Vol. 129, Issue 14
  • DOI: 10.1063/1.2992060

The computer simulation of proton transport in water
journal, November 1999

  • Schmitt, Udo W.; Voth, Gregory A.
  • The Journal of Chemical Physics, Vol. 111, Issue 20
  • DOI: 10.1063/1.480032

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

  • Chaimovich, Aviel; Shell, M. Scott
  • The Journal of Chemical Physics, Vol. 134, Issue 9
  • DOI: 10.1063/1.3557038

Flexible simple point-charge water model with improved liquid-state properties
journal, January 2006

  • Wu, Yujie; Tepper, Harald L.; Voth, Gregory A.
  • The Journal of Chemical Physics, Vol. 124, Issue 2
  • DOI: 10.1063/1.2136877

Modeling Molecular Interactions in Water: From Pairwise to Many-Body Potential Energy Functions
journal, May 2016

  • Cisneros, Gerardo Andrés; Wikfeldt, Kjartan Thor; Ojamäe, Lars
  • Chemical Reviews, Vol. 116, Issue 13
  • DOI: 10.1021/acs.chemrev.5b00644

Development of a “First-Principles” Water Potential with Flexible Monomers. III. Liquid Phase Properties
journal, July 2014

  • Medders, Gregory R.; Babin, Volodymyr; Paesani, Francesco
  • Journal of Chemical Theory and Computation, Vol. 10, Issue 8
  • DOI: 10.1021/ct5004115

The missing term in effective pair potentials
journal, November 1987

  • Berendsen, H. J. C.; Grigera, J. R.; Straatsma, T. P.
  • The Journal of Physical Chemistry, Vol. 91, Issue 24
  • DOI: 10.1021/j100308a038

A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
journal, April 2010

  • Grimme, Stefan; Antony, Jens; Ehrlich, Stephan
  • The Journal of Chemical Physics, Vol. 132, Issue 15
  • DOI: 10.1063/1.3382344

Effects of the dispersion interaction in liquid water
journal, September 2011

Role of Presolvation and Anharmonicity in Aqueous Phase Hydrated Proton Solvation and Transport
journal, November 2015

  • Biswas, Rajib; Tse, Ying-Lung Steve; Tokmakoff, Andrei
  • The Journal of Physical Chemistry B, Vol. 120, Issue 8
  • DOI: 10.1021/acs.jpcb.5b09466

The Curious Case of the Hydrated Proton
journal, August 2011

  • Knight, Chris; Voth, Gregory A.
  • Accounts of Chemical Research, Vol. 45, Issue 1
  • DOI: 10.1021/ar200140h

Perspective: How good is DFT for water?
journal, April 2016

  • Gillan, Michael J.; Alfè, Dario; Michaelides, Angelos
  • The Journal of Chemical Physics, Vol. 144, Issue 13
  • DOI: 10.1063/1.4944633

Multiscale reactive molecular dynamics
journal, December 2012

  • Knight, Chris; Lindberg, Gerrick E.; Voth, Gregory A.
  • The Journal of Chemical Physics, Vol. 137, Issue 22
  • DOI: 10.1063/1.4743958
    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    Recent advances in quantum‐mechanical molecular dynamics simulations of proton transfer mechanism in various water‐based environments
    journal, May 2019

    • Sakti, Aditya W.; Nishimura, Yoshifumi; Nakai, Hiromi
    • WIREs Computational Molecular Science, Vol. 10, Issue 1
    • DOI: 10.1002/wcms.1419

    Correlated dynamics in aqueous proton diffusion
    journal, January 2018

    • Fischer, Sean A.; Dunlap, Brett I.; Gunlycke, Daniel
    • Chemical Science, Vol. 9, Issue 35
    • DOI: 10.1039/c8sc01253a

    Correlated Dynamics in Aqueous Proton Diffusion
    text, January 2018

    Correlated dynamics in aqueous proton diffusion
    journal, January 2018

    • Fischer, Sean A.; Dunlap, Brett I.; Gunlycke, Daniel
    • Chemical Science, Vol. 9, Issue 35
    • DOI: 10.1039/c8sc01253a
      Sort by:
      [ × clear filter / sort ]

      Figures / Tables found in this record:

      FIG. 1 (p. 5)figure
      FIG. 2 (p. 6)figure
      FIG. 3 (p. 7)figure
      FIG. 4 (p. 7)figure
        [ × clear filter / sort ]
        Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

        Similar Records in DOE PAGES and OSTI.GOV collections: