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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 here 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]
  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) (SC-22); National Natural Science Foundation of China (NNSFC); China Scholarship Council
OSTI Identifier:
1512315
Alternate Identifier(s):
OSTI ID: 1373443; OSTI ID: 1512937
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.
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. doi:10.1063/1.4985903.
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. doi:10.1063/1.4985903. https://www.osti.gov/servlets/purl/1512315.
@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 here 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 = {2017},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 3 works
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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.

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.