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The rapid development of universal machine learning potentials (uMLPs) has enabled efficient, accurate predictions of diverse material properties across broad chemical spaces. While their capability for modeling phonon properties is emerging, systematic benchmarking across chemically diverse systems remains limited. We evaluate six recent uMLPs—EquiformerV2, MatterSim, MACE, and CHGNet—on 2429 crystalline materials from the Open Quantum Materials Database. Models were used to compute atomic forces in displaced supercells, derive interatomic force constants (IFCs), and predict phonon properties including lattice thermal conductivity (LTC), compared with density functional theory and experimental data. The EquiformerV2 pretrained model trained on the OMat24 dataset exhibits strong performance in predicting atomic forces and third‐order IFCs, while its fine‐tuned counterpart consistently outperforms other models in predicting second‐order IFCs, LTC, and other phonon properties. Although MACE and CHGNet demonstrated comparable force prediction accuracy to EquiformerV2, notable discrepancies in IFC fitting led to poor LTC predictions. Conversely, MatterSim, despite lower force accuracy, achieved intermediate IFC predictions, suggesting error cancellation and complex relationships between force accuracy and phonon predictions. This benchmark guides the evaluation and selection of uMLPs for high‐throughput screening of materials with targeted thermal transport properties.
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This content will become publicly available on June 30, 2027
Probing Machine Learning Interatomic Potentials on Ion Transport Properties
Machine learning interatomic potentials (MLPs) are promising for accelerating the simulation of ion transport in all‐solid‐state battery materials, but their accuracy across diverse material compositions and symmetries remains unquantified. Here, we systematically benchmark six state‐of‐the‐art MLPs, namely CHGNet, EquiformerV2 in two training variants, MatterSim, SevenNet, and MACE, on representative Li‐ and Na‐based superionic conductors. By comparing predicted atomic forces, diffusion coefficients (DCs) from MLP‐driven molecular dynamics simulations, and second‐ and third‐order interatomic force constants (IFCs) against density functional theory (DFT) and ab initio molecular dynamics (AIMD), we assess the predictive reliability of each model across these properties. EquiformerV2 models, especially the variant trained only on the OMAT dataset, exhibit the lowest force prediction errors and yield DCs in the closest agreement with AIMD. Continually, MLPs with more accurate force predictions produce more reliable diffusion metrics. However, while second‐order IFCs are reasonably captured, all models struggle to reproduce third‐order (anharmonic) IFCs, highlighting significant challenges in modeling anharmonic lattice dynamics with current MLPs. This benchmark study highlights the importance of accurately capturing atomic forces in reasonably producing ion transport properties in all‐solid‐state battery materials and provides practical guidance for universal MLP selection for ion transport simulations and future improvement and development.
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- PAR ID:
- 10702909
- Publisher / Repository:
- Wiley
- Date Published:
- Journal Name:
- Advanced Intelligent Discovery
- ISSN:
- 2943-9981
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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