Constructing multicomponent cluster expansions with machine-learning and chemical embedding

Abstract Cluster expansions are commonly employed as surrogate models to link the electronic structure of an alloy to its finite-temperature properties. Using cluster expansions to model materials with several alloying elements is challenging due to a rapid increase in the number of fitting paramete...

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Main Authors: Yann L. Müller, Anirudh Raju Natarajan
Format: Article
Language:English
Published: Nature Portfolio 2025-03-01
Series:npj Computational Materials
Online Access:https://doi.org/10.1038/s41524-025-01543-3
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author Yann L. Müller
Anirudh Raju Natarajan
author_facet Yann L. Müller
Anirudh Raju Natarajan
author_sort Yann L. Müller
collection DOAJ
description Abstract Cluster expansions are commonly employed as surrogate models to link the electronic structure of an alloy to its finite-temperature properties. Using cluster expansions to model materials with several alloying elements is challenging due to a rapid increase in the number of fitting parameters and training set size. We introduce the embedded cluster expansion (eCE) formalism that enables the parameterization of accurate on-lattice surrogate models for alloys containing several chemical species. The eCE model simultaneously learns a low dimensional embedding of site basis functions along with the weights of an energy model. A prototypical senary alloy comprised of elements in groups 5 and 6 of the periodic table is used to demonstrate that eCE models can accurately reproduce ordering energetics of complex alloys without a significant increase in model complexity. Further, eCE models can leverage similarities between chemical elements to efficiently extrapolate into compositional spaces that are not explicitly included in the training dataset. The eCE formalism presented in this study unlocks the possibility of employing cluster expansion models to study multicomponent alloys containing several alloying elements.
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spelling doaj-art-9424e3ec76604eddbfefec252d13c04f2025-08-20T01:57:48ZengNature Portfolionpj Computational Materials2057-39602025-03-0111111110.1038/s41524-025-01543-3Constructing multicomponent cluster expansions with machine-learning and chemical embeddingYann L. Müller0Anirudh Raju Natarajan1Laboratory of materials design and simulation (MADES), Institute of Materials, École Polytechnique Fédérale de LausanneLaboratory of materials design and simulation (MADES), Institute of Materials, École Polytechnique Fédérale de LausanneAbstract Cluster expansions are commonly employed as surrogate models to link the electronic structure of an alloy to its finite-temperature properties. Using cluster expansions to model materials with several alloying elements is challenging due to a rapid increase in the number of fitting parameters and training set size. We introduce the embedded cluster expansion (eCE) formalism that enables the parameterization of accurate on-lattice surrogate models for alloys containing several chemical species. The eCE model simultaneously learns a low dimensional embedding of site basis functions along with the weights of an energy model. A prototypical senary alloy comprised of elements in groups 5 and 6 of the periodic table is used to demonstrate that eCE models can accurately reproduce ordering energetics of complex alloys without a significant increase in model complexity. Further, eCE models can leverage similarities between chemical elements to efficiently extrapolate into compositional spaces that are not explicitly included in the training dataset. The eCE formalism presented in this study unlocks the possibility of employing cluster expansion models to study multicomponent alloys containing several alloying elements.https://doi.org/10.1038/s41524-025-01543-3
spellingShingle Yann L. Müller
Anirudh Raju Natarajan
Constructing multicomponent cluster expansions with machine-learning and chemical embedding
npj Computational Materials
title Constructing multicomponent cluster expansions with machine-learning and chemical embedding
title_full Constructing multicomponent cluster expansions with machine-learning and chemical embedding
title_fullStr Constructing multicomponent cluster expansions with machine-learning and chemical embedding
title_full_unstemmed Constructing multicomponent cluster expansions with machine-learning and chemical embedding
title_short Constructing multicomponent cluster expansions with machine-learning and chemical embedding
title_sort constructing multicomponent cluster expansions with machine learning and chemical embedding
url https://doi.org/10.1038/s41524-025-01543-3
work_keys_str_mv AT yannlmuller constructingmulticomponentclusterexpansionswithmachinelearningandchemicalembedding
AT anirudhrajunatarajan constructingmulticomponentclusterexpansionswithmachinelearningandchemicalembedding