Optimization of Empirical Force Fields by Parameter Space Mapping: A Single-Step Perturbation Approach

© 2017 American Chemical Society. A general method for parametrizing atomic interaction functions is presented. The method is based on an analysis of surfaces corresponding to the difference between calculated and target data as a function of alternative combinations of parameters (parameter space m...

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Main Authors: Stroet, M., Koziara, Kasia, Malde, A., Mark, A.
Format: Journal Article
Published: American Chemical Society 2017
Online Access:http://hdl.handle.net/20.500.11937/72616
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author Stroet, M.
Koziara, Kasia
Malde, A.
Mark, A.
author_facet Stroet, M.
Koziara, Kasia
Malde, A.
Mark, A.
author_sort Stroet, M.
building Curtin Institutional Repository
collection Online Access
description © 2017 American Chemical Society. A general method for parametrizing atomic interaction functions is presented. The method is based on an analysis of surfaces corresponding to the difference between calculated and target data as a function of alternative combinations of parameters (parameter space mapping). The consideration of surfaces in parameter space as opposed to local values or gradients leads to a better understanding of the relationships between the parameters being optimized and a given set of target data. This in turn enables for a range of target data from multiple molecules to be combined in a robust manner and for the optimal region of parameter space to be trivially identified. The effectiveness of the approach is illustrated by using the method to refine the chlorine 6-12 Lennard-Jones parameters against experimental solvation free enthalpies in water and hexane as well as the density and heat of vaporization of the liquid at atmospheric pressure for a set of 10 aromatic-chloro compounds simultaneously. Single-step perturbation is used to efficiently calculate solvation free enthalpies for a wide range of parameter combinations. The capacity of this approach to parametrize accurate and transferrable force fields is discussed.
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spelling curtin-20.500.11937-726162018-12-13T09:34:51Z Optimization of Empirical Force Fields by Parameter Space Mapping: A Single-Step Perturbation Approach Stroet, M. Koziara, Kasia Malde, A. Mark, A. © 2017 American Chemical Society. A general method for parametrizing atomic interaction functions is presented. The method is based on an analysis of surfaces corresponding to the difference between calculated and target data as a function of alternative combinations of parameters (parameter space mapping). The consideration of surfaces in parameter space as opposed to local values or gradients leads to a better understanding of the relationships between the parameters being optimized and a given set of target data. This in turn enables for a range of target data from multiple molecules to be combined in a robust manner and for the optimal region of parameter space to be trivially identified. The effectiveness of the approach is illustrated by using the method to refine the chlorine 6-12 Lennard-Jones parameters against experimental solvation free enthalpies in water and hexane as well as the density and heat of vaporization of the liquid at atmospheric pressure for a set of 10 aromatic-chloro compounds simultaneously. Single-step perturbation is used to efficiently calculate solvation free enthalpies for a wide range of parameter combinations. The capacity of this approach to parametrize accurate and transferrable force fields is discussed. 2017 Journal Article http://hdl.handle.net/20.500.11937/72616 10.1021/acs.jctc.7b00800 American Chemical Society restricted
spellingShingle Stroet, M.
Koziara, Kasia
Malde, A.
Mark, A.
Optimization of Empirical Force Fields by Parameter Space Mapping: A Single-Step Perturbation Approach
title Optimization of Empirical Force Fields by Parameter Space Mapping: A Single-Step Perturbation Approach
title_full Optimization of Empirical Force Fields by Parameter Space Mapping: A Single-Step Perturbation Approach
title_fullStr Optimization of Empirical Force Fields by Parameter Space Mapping: A Single-Step Perturbation Approach
title_full_unstemmed Optimization of Empirical Force Fields by Parameter Space Mapping: A Single-Step Perturbation Approach
title_short Optimization of Empirical Force Fields by Parameter Space Mapping: A Single-Step Perturbation Approach
title_sort optimization of empirical force fields by parameter space mapping: a single-step perturbation approach
url http://hdl.handle.net/20.500.11937/72616