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

Title: Combining configurational energies and forces for molecular force field optimization

Abstract

While quantum chemical simulations have been increasingly used as an invaluable source of information for atomistic model development, the high computational expenses typically associated with these techniques often limit thorough sampling of the systems of interest. It is therefore of great practical importance to use all available information as efficiently as possible, and in a way that allows for consistent addition of constraints that may be provided by macroscopic experiments. Here we propose a simple approach that combines information from configurational energies and forces generated in a molecular dynamics simulation to increase the effective number of samples. Subsequently, this information is used to optimize a molecular force field by minimizing the statistical distance similarity metric. We illustrate the methodology on an example of a trajectory of configurations generated in equilibrium molecular dynamics simulations of argon and water and compare the results with those based on the force matching method.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]
+ Show Author Affiliations
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division, Joint Inst. for Computational Sciences
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Material Sciences; Vanderbilt Univ., Nashville, TN (United States). Dept. of Chemical and Biomolecular Engineering
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Material Sciences, Computer Science and Mathematics Division
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1399375
Alternate Identifier(s):
OSTI ID: 1372121
Grant/Contract Number:  
AC05-00OR22725
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:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Vlcek, Lukas, Sun, Weiwei, and Kent, Paul R. C. Combining configurational energies and forces for molecular force field optimization. United States: N. p., 2017. Web. doi:10.1063/1.4986079.
Copy to clipboard
Vlcek, Lukas, Sun, Weiwei, & Kent, Paul R. C. Combining configurational energies and forces for molecular force field optimization. United States. https://doi.org/10.1063/1.4986079
Copy to clipboard
Vlcek, Lukas, Sun, Weiwei, and Kent, Paul R. C. Fri . "Combining configurational energies and forces for molecular force field optimization". United States. https://doi.org/10.1063/1.4986079. https://www.osti.gov/servlets/purl/1399375.
Copy to clipboard
@article{osti_1399375,
title = {Combining configurational energies and forces for molecular force field optimization},
author = {Vlcek, Lukas and Sun, Weiwei and Kent, Paul R. C.},
abstractNote = {While quantum chemical simulations have been increasingly used as an invaluable source of information for atomistic model development, the high computational expenses typically associated with these techniques often limit thorough sampling of the systems of interest. It is therefore of great practical importance to use all available information as efficiently as possible, and in a way that allows for consistent addition of constraints that may be provided by macroscopic experiments. Here we propose a simple approach that combines information from configurational energies and forces generated in a molecular dynamics simulation to increase the effective number of samples. Subsequently, this information is used to optimize a molecular force field by minimizing the statistical distance similarity metric. We illustrate the methodology on an example of a trajectory of configurations generated in equilibrium molecular dynamics simulations of argon and water and compare the results with those based on the force matching method.},
doi = {10.1063/1.4986079},
journal = {Journal of Chemical Physics},
number = 16,
volume = 147,
place = {United States},
year = {Fri Jul 21 00:00:00 EDT 2017},
month = {Fri Jul 21 00:00:00 EDT 2017}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1063/1.4986079
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 11 works
Citation information provided by
Web of Science
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:

The Geometry of Asymptotic Inference
journal, August 1989

Effective force fields for condensed phase systems from ab initio molecular dynamics simulation: A new method for force-matching
journal, June 2004

  • Izvekov, Sergei; Parrinello, Michele; Burnham, Christian J.
  • The Journal of Chemical Physics, Vol. 120, Issue 23
  • DOI: 10.1063/1.1739396

The force matching approach to multiscale simulations: Merits, shortcomings, and future perspectives
journal, February 2014

  • Masia, Marco; Guàrdia, Elvira; Nicolini, Paolo
  • International Journal of Quantum Chemistry, Vol. 114, Issue 16
  • DOI: 10.1002/qua.24621

Statistical distance and the geometry of quantum states
journal, May 1994

Efficient estimation of free energy differences from Monte Carlo data
journal, October 1976

Derivation of coarse-grained potentials via multistate iterative Boltzmann inversion
journal, June 2014

  • Moore, Timothy C.; Iacovella, Christopher R.; McCabe, Clare
  • The Journal of Chemical Physics, Vol. 140, Issue 22
  • DOI: 10.1063/1.4880555

On the binding of nanometric hydrogen–helium clusters in tungsten
journal, October 2014

Zur Quantentheorie der Molekeln
journal, January 1927

Interatomic Potentials from First-Principles Calculations: The Force-Matching Method
journal, June 1994

Single-ion hydration thermodynamics from clusters to bulk solutions: Recent insights from molecular modeling
journal, January 2016

Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995

Derivation of class II force fields. I. Methodology and quantum force field for the alkyl functional group and alkane molecules
journal, February 1994

  • Maple, J. R.; Hwang, M. -J.; Stockfisch, T. P.
  • Journal of Computational Chemistry, Vol. 15, Issue 2
  • DOI: 10.1002/jcc.540150207

ReaxFF:  A Reactive Force Field for Hydrocarbons
journal, October 2001

  • van Duin, Adri C. T.; Dasgupta, Siddharth; Lorant, Francois
  • The Journal of Physical Chemistry A, Vol. 105, Issue 41
  • DOI: 10.1021/jp004368u

A Polarizable and Transferable PHAST CO 2 Potential for Materials Simulation
journal, November 2013

  • Mullen, Ashley L.; Pham, Tony; Forrest, Katherine A.
  • Journal of Chemical Theory and Computation, Vol. 9, Issue 12
  • DOI: 10.1021/ct400549q

Optimized Unlike-Pair Interactions for Water–Carbon Dioxide Mixtures Described by the SPC/E and EPM2 Models
journal, July 2011

  • Vlcek, Lukas; Chialvo, Ariel A.; Cole, David R.
  • The Journal of Physical Chemistry B, Vol. 115, Issue 27
  • DOI: 10.1021/jp203241q

Constant Temperature Molecular Dynamics Methods
journal, January 1991

  • Nosé, Shuichi
  • Progress of Theoretical Physics Supplement, Vol. 103
  • DOI: 10.1143/ptps.103.1

A quasi-universal scaling law for atomic transport in simple fluids
journal, January 1999

Interatomic potentials for modelling radiation defects and dislocations in tungsten
journal, September 2013

A modified W–W interatomic potential based on ab initio calculations
journal, December 2013

  • Wang, J.; Zhou, Y. L.; Li, M.
  • Modelling and Simulation in Materials Science and Engineering, Vol. 22, Issue 1
  • DOI: 10.1088/0965-0393/22/1/015004

Systematic coarse-graining of potential energy landscapes and dynamics in liquids
journal, August 2012

  • Shell, M. Scott
  • The Journal of Chemical Physics, Vol. 137, Issue 8
  • DOI: 10.1063/1.4746391

Statistical distance and Hilbert space
journal, January 1981

Rigorous force field optimization principles based on statistical distance minimization
journal, October 2015

  • Vlcek, Lukas; Chialvo, Ariel A.
  • The Journal of Chemical Physics, Vol. 143, Issue 14
  • DOI: 10.1063/1.4932360

A unified formulation of the constant temperature molecular dynamics methods
journal, July 1984

  • Nosé, Shuichi
  • The Journal of Chemical Physics, Vol. 81, Issue 1
  • DOI: 10.1063/1.447334

Deriving effective mesoscale potentials from atomistic simulations: Mesoscale Potentials from Atomistic Simulations
journal, August 2003

  • Reith, Dirk; Pütz, Mathias; Müller-Plathe, Florian
  • Journal of Computational Chemistry, Vol. 24, Issue 13
  • DOI: 10.1002/jcc.10307

The classical equation of state of gaseous helium, neon and argon
journal, October 1938

  • Buckingham, R. A.
  • Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences, Vol. 168, Issue 933, p. 264-283
  • DOI: 10.1098/rspa.1938.0173

The multiscale coarse-graining method. I. A rigorous bridge between atomistic and coarse-grained models
journal, June 2008

  • Noid, W. G.; Chu, Jhih-Wei; Ayton, Gary S.
  • The Journal of Chemical Physics, Vol. 128, Issue 24
  • DOI: 10.1063/1.2938860

Methods of conjugate gradients for solving linear systems
journal, December 1952

  • Hestenes, M. R.; Stiefel, E.
  • Journal of Research of the National Bureau of Standards, Vol. 49, Issue 6
  • DOI: 10.6028/jres.049.044

Water Structure from Scattering Experiments and Simulation
journal, August 2002

  • Head-Gordon, Teresa; Hura, Greg
  • Chemical Reviews, Vol. 102, Issue 8
  • DOI: 10.1021/cr0006831

Building Force Fields: An Automatic, Systematic, and Reproducible Approach
journal, May 2014

  • Wang, Lee-Ping; Martinez, Todd J.; Pande, Vijay S.
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 11
  • DOI: 10.1021/jz500737m
    Sort by:
    [ × clear filter / sort ]

    Similar Records in DOE PAGES and OSTI.GOV collections: