Hybrid ab initio and empirical machine learning models for the potential energy surface

TL;DR

This paper introduces a hybrid machine learning approach that combines ab initio calculations and experimental data to accurately model the potential energy surface, improving the simulation of liquid water properties.

Contribution

A novel hybrid training method that integrates ab initio and experimental data using a combined loss function and reweighting for ensemble averages.

Findings

Accurately reproduces water's density maximum

Replicates experimental density isobar at 1 bar

Matches radial distribution function in simulations

Abstract

We propose a methodology to generate hybrid machine learning models for the potential energy surface trained simultaneously on data from ab initio electronic structure calculations and on thermodynamic and/or structural observables from experiment. The approach is based on the use of a loss function that includes the mean square error of observables with respect to their experimental values, in addition to the usual terms involving the mean square error of the energies and forces with respect to ab initio data. We employ a reweighting procedure that allows for the calculation of ensemble averages of observables during training for arbitrary values of the model parameters and on the fly. The method is general and can be applied to any set of static observables. We illustrate the usefulness of this approach by applying it to the generation of hybrid models for liquid water that reproduce accurately the experimental density maximum, the density isobar at 1 bar, and the radial distribution function in molecular dynamics simulations.