Accelerating CALPHAD-based Phase Diagram Predictions in Complex Alloys Using Universal Machine Learning Potentials: Opportunities and Challenges

TL;DR

This paper demonstrates that machine learning interatomic potentials can drastically accelerate CALPHAD-based phase diagram predictions in complex alloys, enabling high-throughput thermodynamic modeling with maintained accuracy.

Contribution

It introduces a framework combining MLIPs with CALPHAD to significantly speed up phase diagram calculations for complex alloys.

Findings

MLIPs achieve over 1000x speedup compared to DFT.

ORB MLIP maintains acceptable accuracy in phase stability predictions.

The approach is versatile for high-entropy and ternary alloy systems.

Abstract

Accurate phase diagram prediction is crucial for understanding alloy thermodynamics and advancing materials design. While traditional CALPHAD methods are robust, they are resource-intensive and limited by experimentally assessed data. This work explores the use of machine learning interatomic potentials (MLIPs) such as M3GNet, CHGNet, MACE, SevenNet, and ORB to significantly accelerate phase diagram calculations by using the Alloy Theoretic Automated Toolkit (ATAT) to map calculations of the energies and free energies of atomistic systems to CALPHAD-compatible thermodynamic descriptions. Using case studies including Cr-Mo, Cu-Au, and Pt-W, we demonstrate that MLIPs, particularly ORB, achieve computational speedups exceeding three orders of magnitude compared to DFT while maintaining phase stability predictions within acceptable accuracy. Extending this approach to liquid phases and ternary systems like Cr-Mo-V highlights its versatility for high-entropy alloys and complex chemical spaces. This work demonstrates that MLIPs, integrated with tools like ATAT within a CALPHAD framework, provide an efficient and accurate framework for high-throughput thermodynamic modeling, enabling rapid exploration of novel alloy systems. While many challenges remain to be addressed, the accuracy of some of these MLIPs (ORB in particular) are on the verge of paving the way toward high-throughput generation of CALPHAD thermodynamic descriptions of multi-component, multi-phase alloy systems.