Accelerating crystal structure search through active learning with neural networks for rapid relaxations

TL;DR

This paper introduces an active learning approach using neural network force fields to accelerate crystal structure searches, significantly reducing computational costs and effectively identifying stable structures and local minima.

Contribution

The method combines active learning with neural network force fields and uncertainty estimation to drastically reduce the number of steps needed for crystal structure relaxation.

Findings

Reduces computational costs by up to two orders of magnitude

Successfully identifies stable structures in benchmark systems

Finds multiple local minima with minimal additional effort

Abstract

Global optimization of crystal compositions is a significant yet computationally intensive method to identify stable structures within chemical space. The specific physical properties linked to a three-dimensional atomic arrangement make this an essential task in the development of new materials. We present a method that efficiently uses active learning of neural network force fields for structure relaxation, minimizing the required number of steps in the process. This is achieved by neural network force fields equipped with uncertainty estimation, which iteratively guide a pool of randomly generated candidates towards their respective local minima. Using this approach, we are able to effectively identify the most promising candidates for further evaluation using density functional theory (DFT). Our method not only reliably reduces computational costs by up to two orders of magnitude across the benchmark systems Si16 , Na8Cl8 , Ga8As8 and Al4O6 , but also excels in finding the most stable minimum for the unseen, more complex systems Si46 and Al16O24 . Moreover, we demonstrate at the example of Si16 that our method can find multiple relevant local minima while only adding minor computational effort.