title: Fusing heterogeneous data for the calibration of molecular dynamics force fields using hierarchical Bayesian models.
abstract: We propose a hierarchical Bayesian framework to systematically integrate heterogeneous data for the calibration of force fields in Molecular Dynamics (MD) simulations. Our approach enables the fusion of diverse experimental data sets of the physico-chemical properties of a system at different thermodynamic conditions. We demonstrate the value of this framework for the robust calibration of MD force-fields for water using experimental data of its diffusivity, radial distribution function, and density. In order to address the high computational cost associated with the hierarchical Bayesian models, we develop a novel surrogate model based on the empirical interpolation method. Further computational savings are achieved by implementing a highly parallel transitional Markov chain Monte Carlo technique. The present method bypasses possible subjective weightings of the experimental data in identifying MD force-field parameters.
authors.affiliation: Computational Science and Engineering Laboratory, ETH-Zurich, Clausiusstrasse 33, CH-8092 Zurich, Switzerland.
authors.forename: Stephen
authors.initials: S
authors.lastname: Wu
authors.affiliation: Computational Science and Engineering Laboratory, ETH-Zurich, Clausiusstrasse 33, CH-8092 Zurich, Switzerland.
authors.forename: Panagiotis
authors.initials: P
authors.lastname: Angelikopoulos
authors.affiliation: Computational Science and Engineering Laboratory, ETH-Zurich, Clausiusstrasse 33, CH-8092 Zurich, Switzerland.
authors.forename: Gerardo
authors.initials: G
authors.lastname: Tauriello
authors.affiliation: Department of Mechanical Engineering, University of Thessaly, 38334 Volos, Greece.
authors.forename: Costas
authors.initials: C
authors.lastname: Papadimitriou
authors.affiliation: Computational Science and Engineering Laboratory, ETH-Zurich, Clausiusstrasse 33, CH-8092 Zurich, Switzerland.
authors.forename: Petros
authors.initials: P
authors.lastname: Koumoutsakos