Expanding the search space of high entropy oxides and predicting synthesizability using machine learning interatomic potentials

TL;DR

This paper introduces a machine learning-based computational method to efficiently predict the synthesizability of high entropy oxides across a vast compositional space, significantly accelerating discovery compared to traditional trial-and-error approaches.

Contribution

It develops a novel approach using machine learned interatomic potentials and entropy/enthalpy descriptors to identify promising high entropy oxide candidates, validated against DFT calculations.

Findings

Successfully identified the only known stable 4-component HEO in a specific structure.

Predicted several new 5-component HEO candidates.

Validated the approach with DFT comparisons for 7 elements.

Abstract

We propose an efficient computational methodology for predicting the synthesizability of high entropy oxides (HEOs) in a large space of possible candidate compounds. HEOs are a growing field with an enormous potential chemical composition space, and yet the discovery of new HEOs is slow and driven by experimental trial-and-error. In this work, we attempt to speed up this process by using a machine learned interatomic potential offering DFT-level accuracy. Our methodology starts by identifying a set of crystal structures and elements for screening, building a large random unit cell of each composition and structure, then relaxing this structure. The most promising candidates are distinguished based on the variance of the individual cation energies, which we introduce as our entropy descriptor, and the enthalpy of mixing, which is used as the enthalpy descriptor. The approach is applied to tetravalent HEOs, and its validity is confirmed by comparison to alternative descriptors and DFT calculations for a set of 7 elements. The search is then extended to a set of 14 elements and three crystal structures, where it successfully identifies the only known stable 4-component HEO in the $\alpha$-PbO$_2$ structure, as well as predicting several new 5-component candidate systems. This approach can straightforwardly be applied to new sets of elements and structures, allowing for the accelerated discovery of new HEOs.