Benchmarking CHGNet Universal Machine Learning Interatomic Potential Against DFT and EXAFS: Case of Layered WS2 and MoS2

Abstract

Universal machine learning interatomic potentials (uMLIPs) deliver near ab initio accuracy in energy and force calculations at low computational cost, making them invaluable for materials modeling. Although uMLIPs are pre-trained on vast ab initio datasets, rigorous validation remains essential for their ongoing adoption. In this study, we use the CHGNet uMLIP to model thermal disorder in isostructural layered 2Hc-WS2 and 2Hc-MoS2, benchmarking it against ab initio data and extended X-ray absorption fine structure (EXAFS) spectra, which capture thermal variations in bond lengths and angles. Fine-tuning CHGNet with compound-specific ab initio (DFT) data mitigates the systematic softening (i.e., force underestimation) typical of uMLIPs and simultaneously improves alignment between molecular dynamics-derived and experimental EXAFS spectra. While fine-tuning with a single DFT structure is viable, using ~100 structures is recommended to accurately reproduce EXAFS spectra and achieve DFT-level accuracy. Benchmarking the CHGNet uMLIP against both DFT and experimental EXAFS data reinforces confidence in its performance and provides guidance for determining optimal fine-tuning dataset sizes.

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