Application of the ChIMES Force Field to Nonreactive Molecular Systems: Water at Ambient Conditions

Lindsey, Rebecca K.; Fried, Laurence E.; Goldman, Nir

doi:10.1021/acs.jctc.8b00831

Title: Application of the ChIMES Force Field to Nonreactive Molecular Systems: Water at Ambient Conditions

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Abstract

We demonstrate development of the Chebyshev Interaction Model for Efficient Simulation (ChIMES) for molecular systems through application to water under ambient conditions (298 K, 1 g/cm³). These models, which are comprised of linear combinations of Chebyshev polynomials explicitly describing two- and three-body interactions, are largely fit by force matching to Kohn–Sham Density Functional Theory (DFT). Protocols for selecting user-specified parameters and inclusion of stress tensor data are investigated, and structural and dynamical property prediction for resulting models is benchmarked against DFT. We show that the present ChIMES force fields yield excellent agreement with DFT without the need for additional terms such as those for Coulomb interactions. Overall, we show that tractable parametrization and subsequent accuracy of the present models make ChIMES an ideal candidate for extension of DFT dynamics to larger system sizes and longer time scales.

Authors:

^[1];

^[2]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Physical and Life Sciences Directorate
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Physical and Life Sciences Directorate; Univ. of California, Davis, CA (United States). Dept. of Chemical Engineering

Publication Date:: Mon Nov 26 00:00:00 EST 2018

Research Org.:: Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1512587

Report Number(s):: LLNL-JRNL-756242
Journal ID: ISSN 1549-9618; 943657

Grant/Contract Number:: AC52-07NA27344

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Chemical Theory and Computation

Additional Journal Information:: Journal Volume: 15; Journal Issue: 1; Journal ID: ISSN 1549-9618

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Lindsey, Rebecca K., Fried, Laurence E., and Goldman, Nir. Application of the ChIMES Force Field to Nonreactive Molecular Systems: Water at Ambient Conditions.  United States: N. p., 2018. 
Web.  doi:10.1021/acs.jctc.8b00831.

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                    Lindsey, Rebecca K., Fried, Laurence E., & Goldman, Nir. Application of the ChIMES Force Field to Nonreactive Molecular Systems: Water at Ambient Conditions.  United States.  https://doi.org/10.1021/acs.jctc.8b00831

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                    Lindsey, Rebecca K., Fried, Laurence E., and Goldman, Nir. Mon .  
"Application of the ChIMES Force Field to Nonreactive Molecular Systems: Water at Ambient Conditions".  United States.  https://doi.org/10.1021/acs.jctc.8b00831.  https://www.osti.gov/servlets/purl/1512587.

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@article{osti_1512587,

  title        = {Application of the ChIMES Force Field to Nonreactive Molecular Systems: Water at Ambient Conditions},

  author       = {Lindsey, Rebecca K. and Fried, Laurence E. and Goldman, Nir},

  abstractNote = {We demonstrate development of the Chebyshev Interaction Model for Efficient Simulation (ChIMES) for molecular systems through application to water under ambient conditions (298 K, 1 g/cm3). These models, which are comprised of linear combinations of Chebyshev polynomials explicitly describing two- and three-body interactions, are largely fit by force matching to Kohn–Sham Density Functional Theory (DFT). Protocols for selecting user-specified parameters and inclusion of stress tensor data are investigated, and structural and dynamical property prediction for resulting models is benchmarked against DFT. We show that the present ChIMES force fields yield excellent agreement with DFT without the need for additional terms such as those for Coulomb interactions. Overall, we show that tractable parametrization and subsequent accuracy of the present models make ChIMES an ideal candidate for extension of DFT dynamics to larger system sizes and longer time scales.},

  doi          = {10.1021/acs.jctc.8b00831},

  journal      = {Journal of Chemical Theory and Computation},

  number       = 1,

  volume       = 15,

  place        = {United States},

  year         = {Mon Nov 26 00:00:00 EST 2018},

  month        = {Mon Nov 26 00:00:00 EST 2018}

}

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