Quantifying Parameter Sensitivity and Uncertainty for Interatomic Potential Design: Application to Saturated Hydrocarbons

The research objective herein is to understand the relationships between the interatomic potential parameters and properties used in the training and validation of potentials, specifically using a recently developed modified embedded-atom method (MEAM) potential for saturated hydrocarbons (C–H system). This potential was parameterized to a training set that included bond distances, bond angles, and atomization energies at 0 K of a series of alkane structures from methane to n-octane. In this work, the parameters of the MEAM potential were explored through a fractional factorial design and a Latin hypercube design to better understand how individual MEAM parameters affected several properties of molecules (energy, bond distances, bond angles, and dihedral angles) and also to quantify the relationship/correlation between various molecules in terms of these properties. The generalized methodology presented shows quantitative approaches that can be used in selecting the appropriate parameters for the interatomic potential, selecting the bounds for these parameters (for constrained optimization), selecting the responses for the training set, selecting the weights for various responses in the objective function, and setting up the single/multi-objective optimization process itself. The significance of the approach applied in this study is not only the application to the C–H system but that the broader framework can also be easily applied to any number of systems to understand the significance of parameters, their relationships to properties, and the subsequent steps for designing interatomic potentials under uncertainty.