Optimization of Transferable Interatomic Potentials for Glasses toward Experimental Properties

Abstract

The accuracy of molecular simulations is fundamentally limited by the interatomic potentials that govern atomic interactions. Traditional potential development, which relies heavily on ab initio calculations, frequently struggles to reproduce the experimentally observed properties that govern real material behavior. To address this challenge, we present a machine learning-driven, active-learning optimization framework for optimizing classical interatomic potentials to reproduce experimental properties. Our method, here showcased on soda-lime borosilicate glasses, targets both global (density) and local (boron coordination) structural features across a wide range of compositions. By combining a surrogate model with iterative active learning, the framework efficiently explores a five-dimensional parameter space using only 400 molecular dynamics simulations over 17 iterations, making it highly data-efficient and eliminating the need for extensive simulation campaigns. Two transferable parameter sets are identified, each demonstrating good agreement with experimental measurements, including glass density, fraction of four-fold boron, and X-ray structure factor. The framework effectively captures and manages inherent trade-offs between structural objectives and compositional regimes, providing insights into the coordination behavior of boron in complex glass networks. The resulting classical force fields are generalizable and do not require reparameterization for individual compositions. Altogether, this work offers a scalable and experimentally grounded approach for developing transferable interatomic potentials suitable for a broad range of materials, including multi-component glass systems, and beyond.