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The Journal of Chemical Physics
Article . 2025 . Peer-reviewed
License: CC BY
Data sources: Crossref
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https://dx.doi.org/10.48550/ar...
Article . 2024
License: CC BY
Data sources: Datacite
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Accuracy of charge densities in electronic structure calculations

Authors: Moritz Gubler; Moritz R. Schäfer; Jörg Behler; Stefan Goedecker;

Accuracy of charge densities in electronic structure calculations

Abstract

Accurate charge densities are essential for reliable electronic structure calculations because they significantly impact predictions of various chemical properties and, in particular, according to the Hellmann–Feynman theorem, atomic forces. This study examines the accuracy of charge densities obtained from different density functional theory (DFT) exchange–correlation functionals in comparison with coupled cluster calculations with single and double excitations. We find that modern DFT functionals can provide highly accurate charge densities, particularly in case of meta-generalized gradient approximations and hybrid functionals. In connection with Gaussian basis sets, it is necessary to use the largest basis sets available to obtain densities that are nearly free of basis set errors. These findings highlight the importance of selecting appropriate computational methods for generating high-precision charge densities, which are, for instance, needed to generate reference data for training modern machine learned potentials.

Keywords

Chemical Physics (physics.chem-ph), Physics - Chemical Physics, FOS: Physical sciences

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selected citations
These citations are derived from selected sources.
This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Citations provided by BIP!
popularity
This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
BIP!Popularity provided by BIP!
influence
This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Influence provided by BIP!
impulse
This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
BIP!Impulse provided by BIP!
12
Top 10%
Top 10%
Top 10%
Green
hybrid