Hydrogen, Oxygen, and Lead Adsorbates on Al 13 Co 4 (100): Accurate Potential Energy Surfaces at Low Computational Cost by Machine Learning and DFT-Based Data - Archive ouverte HAL
Article Dans Une Revue Journal of Chemical Theory and Computation Année : 2024

Hydrogen, Oxygen, and Lead Adsorbates on Al 13 Co 4 (100): Accurate Potential Energy Surfaces at Low Computational Cost by Machine Learning and DFT-Based Data

Résumé

Intermetallic compounds are promising materials in numerous fields, especially those involving surface interactions, such as catalysis. A key factor to investigate their surface properties lies in adsorption energy maps, typically built using first-principles approaches. However, exploring the adsorption energy landscapes of intermetallic compounds can be cumbersome, usually requiring huge computational resources. In this work, we propose an efficient method to predict adsorption energies, based on a Machine Learning (ML) scheme fed by a few Density Functional Theory (DFT) estimates performed on n sites selected through the Farthest Point Sampling (FPS) process. We detail its application on the Al13Co4(100) quasicrystalline approximant surface for several atomic adsorbates (H, O, and Pb). On this specific example, our approach is shown to outperform both simple interpolation strategies and the recent ML force field MACE [arXiv.2206.07697], especially when the number n is small, i.e., below 36 sites. The ground-truth DFT adsorption energies are much more correlated with the predicted FPS-ML estimates (Pearson R-factor of 0.71, 0.73, and 0.90 for H, O and Pb, respectively, when n = 36) than with interpolation-based or MACE-ML ones (Pearson R-factors of 0.43, 0.39, and 0.56 for H, O, and Pb, in the former case and 0.22, 0.35, and 0.63 in the latter case). The unbiased root-mean-square error (ubRMSE) is lower for FPS-ML than for interpolation-based and MACE-ML predictions (0.15, 0.17, and 0.17 eV, respectively, for hydrogen and 0.17, 0.25, and 0.22 eV for lead), except for oxygen (0.55, 0.47, and 0.46 eV) due to large surface relaxations in this case. We believe that these findings and the corresponding methodology can be extended to a wide range of systems, which will motivate the discovery of novel functional materials.
Fichier principal
Vignette du fichier
boulangeot24hydrogen.pdf (5.63 Mo) Télécharger le fichier
ct4c00367_si_001.pdf (75.48 Mo) Télécharger le fichier
Origine Fichiers produits par l'(les) auteur(s)

Dates et versions

hal-04759834 , version 1 (07-12-2024)

Identifiants

Citer

Nathan Boulangeot, Florian Brix, Frédéric Sur, Émilie Gaudry. Hydrogen, Oxygen, and Lead Adsorbates on Al 13 Co 4 (100): Accurate Potential Energy Surfaces at Low Computational Cost by Machine Learning and DFT-Based Data. Journal of Chemical Theory and Computation, 2024, 20 (16), pp.7287-7299. ⟨10.1021/acs.jctc.4c00367⟩. ⟨hal-04759834⟩
39 Consultations
0 Téléchargements

Altmetric

Partager

More