Machine Learning Potentials with the Iterative Boltzmann Inversion: Training to Experiment

• Published in: Journal of chemical theory and computation Vol. 20; no. 3; pp. 1274 - 1281
• Main Authors: Matin, Sakib, Allen, Alice E. A., Smith, Justin, Lubbers, Nicholas, Jadrich, Ryan B., Messerly, Richard, Nebgen, Benjamin, Li, Ying Wai, Tretiak, Sergei, Barros, Kipton
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 13-02-2024
• Subjects: Density functional theory; Distribution functions; Iterative methods; Machine learning; Molecular dynamics; Molecular Mechanics; Performance prediction; Radial distribution; Simulation
• ISSN: 1549-9618; 1549-9626
• DOI: 10.1021/acs.jctc.3c01051

Methodologies for training machine learning potentials (MLPs) with quantum-mechanical simulation data have recently seen tremendous progress. Experimental data have a very different character than simulated data, and most MLP training procedures cannot be easily adapted to incorporate both types of data into the training process. We investigate a training procedure based on iterative Boltzmann inversion that produces a pair potential correction to an existing MLP using equilibrium radial distribution function data. By applying these corrections to an MLP for pure aluminum based on density functional theory, we observe that the resulting model largely addresses previous overstructuring in the melt phase. Interestingly, the corrected MLP also exhibits improved performance in predicting experimental diffusion constants, which are not included in the training procedure. The presented method does not require autodifferentiating through a molecular dynamics solver and does not make assumptions about the MLP architecture. Our results suggest a practical framework for incorporating experimental data into machine learning models to improve the accuracy of molecular dynamics simulations.