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The Royal Society, Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, 2060(374), p. 20150032, 2016

DOI: 10.1098/rsta.2015.0032

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A hierarchical Bayesian framework for force field selection in molecular dynamics simulations

Journal article published in 2015 by S. Wu, P. Angelikopoulos ORCID, C. Papadimitriou, R. Moser, P. Koumoutsakos
This paper is made freely available by the publisher.
This paper is made freely available by the publisher.

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Abstract

We present a hierarchical Bayesian framework for the selection of force fields in molecular dynamics (MD) simulations. The framework associates the variability of the optimal parameters of the MD potentials under different environmental conditions with the corresponding variability in experimental data. The high computational cost associated with the hierarchical Bayesian framework is reduced by orders of magnitude through a parallelized Transitional Markov Chain Monte Carlo method combined with the Laplace Asymptotic Approximation. The suitability of the hierarchical approach is demonstrated by performing MD simulations with prescribed parameters to obtain data for transport coefficients under different conditions, which are then used to infer and evaluate the parameters of the MD model. We demonstrate the selection of MD models based on experimental data and verify that the hierarchical model can accurately quantify the uncertainty across experiments; improve the posterior probability density function estimation of the parameters, thus, improve predictions on future experiments; identify the most plausible force field to describe the underlying structure of a given dataset. The framework and associated software are applicable to a wide range of nanoscale simulations associated with experimental data with a hierarchical structure.