A universal machine learning model for the electronic density of states

DOI

<p>In the last few years several ``universal'' interatomic potentials have appeared, using machine-learning approaches to predict energy and forces of atomic configurations with arbitrary composition and structure, with an accuracy often comparable with that of the electronic-structure calculations they are trained on. Here we demonstrate that these generally-applicable models can also be built to predict explicitly the electronic structure of materials and molecules. We focus on the electronic density of states (DOS), and develop PET-MAD-DOS, a rotationally unconstrained transformer model built on the Point Edge Transformer (PET) architecture, and trained on the Massive Atomistic Diversity (MAD) dataset. We demonstrate our model's predictive abilities on samples from diverse external datasets, showing also that the DOS can be further manipulated to obtain accurate band gap predictions. A fast evaluation of the DOS is especially useful in combination with molecular simulations probing matter in finite-temperature thermodynamic conditions. To assess the accuracy of PET-MAD-DOS in this context, we evaluate the ensemble-averaged DOS and the electronic heat capacity of three technologically relevant systems: lithium thiophosphate (LPS), gallium arsenide (GaAs), and a high entropy alloy (HEA). By comparing with bespoke models, trained exclusively on system-specific datasets, we show that our universal model achieves semi-quantitative agreement for all these tasks. Furthermore, we demonstrate that fine-tuning can be performed using a small fraction of the bespoke data, yielding models that are comparable to, and sometimes better than, fully-trained bespoke models. </p>

Identifier
DOI https://doi.org/10.24435/materialscloud:gs-z7
Related Identifier https://doi.org/10.48550/arXiv.2508.17418
Related Identifier https://archive.materialscloud.org/communities/mcarchive
Related Identifier https://doi.org/10.24435/materialscloud:7e-17
Metadata Access https://archive.materialscloud.org/oai2d?verb=GetRecord&metadataPrefix=oai_dc&identifier=oai:materialscloud.org:8ee9k-b7865
Provenance
Creator How, Wei Bin; Febrer, Pol; Chong, Sanggyu; Mazitov, Arslan; Bigi, Filippo; Kellner, Matthias; Pozdnyakov, Sergey; Ceriotti, Michele
Publisher Materials Cloud
Contributor Ceriotti, Michele
Publication Year 2025
Rights info:eu-repo/semantics/openAccess; Creative Commons Attribution 4.0 International; https://creativecommons.org/licenses/by/4.0/legalcode
OpenAccess true
Contact archive(at)materialscloud.org
Representation
Language English
Resource Type info:eu-repo/semantics/other
Format text/markdown; application/gzip
Discipline Materials Science and Engineering