title: Statistical approaches to forcefield calibration and prediction uncertainty in molecular simulation.
abstract: Calibration of forcefields for molecular simulation should account for the measurement uncertainty of the reference dataset and for the model inadequacy, i.e., the inability of the force-field/simulation pair to reproduce experimental data within their uncertainty range. In all rigour, the resulting uncertainty of calibrated force-field parameters is a source of uncertainty for simulation predictions. Various calibration strategies and calibration models within the Bayesian calibration/prediction framework are explored in the present article. In the case of Lennard-Jones potential for Argon, we show that prediction uncertainty for thermodynamical and transport properties, albeit very small, is larger than statistical simulation uncertainty.
authors.affiliation: Laboratoire de Chimie Physique, UMR8000, CNRS/Univ. Paris-Sud, 91405 Orsay, France. fabien.cailliez@u-psud.fr
authors.forename: Fabien
authors.initials: F
authors.lastname: Cailliez
authors.forename: Pascal
authors.initials: P
authors.lastname: Pernot