Bayesian optimization of atomic structures with prior probabilities from universal interatomic potentials

TL;DR

This paper introduces a Bayesian optimization method that leverages universal machine learning potentials as priors to efficiently find atomic structures, significantly reducing computational effort in complex energy landscapes.

Contribution

It presents a novel combination of universal machine learning potentials with Gaussian process Bayesian optimization, improving the speed of atomic structure determination.

Findings

Faster identification of global minima in atomic structures.

Effective across diverse systems like bulk materials, surfaces, and clusters.

Enhanced efficiency over traditional methods.

Abstract

The optimization of atomic structures plays a pivotal role in understanding and designing materials with desired properties. However, conventional computational methods often struggle with the formidable task of navigating the vast potential energy surface, especially in high-dimensional spaces with numerous local minima. Recent advancements in machine learning-driven surrogate models offer a promising avenue for alleviating this computational burden. In this study, we propose a novel approach that combines the strengths of universal machine learning potentials with a Bayesian approach using Gaussian processes. By using the machine learning potentials as priors for the Gaussian process, the Gaussian process has to learn only the difference between the machine learning potential and the target energy surface calculated for example by density functional theory. This turns out to improve the speed by which the global optimal structure is identified across diverse systems for a well-behaved machine learning potential. The approach is tested on periodic bulk materials, surface structures, and a cluster.