Comparing Hubbard parameters from linear-response theory and a Hartree-Fock-based approach
- 1. Korea Institute for Advanced Study, Seoul 02455, Republic of Korea
- 2. Oden Institute for Computational Engineering and Sciences, The University of Texas at Austin, Austin, Texas 78712, USA
- 3. PSI Center for Scientific Computing, Theory and Data, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
- 4. Open MOLCAS Community, Geneva 1219, Switzerland
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Description
Density-functional theory with on-site U and inter-site V Hubbard corrections (DFT+U+V) is widely used to predict properties of transition-metal and rare-earth compounds, but its accuracy depends critically on how these parameters are obtained. While they can be determined empirically, first-principles approaches offer better consistency, though their results can differ and a systematic comparison is lacking. Here, we compare two widely used approaches, linear-response theory (LRT) and the Hartree–Fock-based pseudohybrid functional formalism, applied to representative oxides (MnO, NiO, CoO, FeO, BaTiO3, ZnO, and ZrO2). For partially occupied transition-metal d states, both methods yield comparable U values, but they differ significantly for nearly empty or fully filled d shells. For O-2p states, LRT systematically predicts large U values (~10 eV), whereas the pseudohybrid approach gives system-dependent values. Even larger differences appear for the inter-site V: the former yields small values (<1 eV), while the latter gives larger values (~3 eV) due to its dependence on charge redistribution. We further show that the pseudopotential choice, which defines Hubbard projectors, affects the parameters and their agreement. Overall, while parallels between these two methods exist, they rely on different assumptions, leading to variations in predictions of material properties.
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Funding
- Discovery, design, and characterization of novel Na-ion cathode battery materials 200021-227641
- Swiss National Science Foundation
- Harnessing chiral magnons in altermagnets via advanced computational methods 200021-236507
- Swiss National Science Foundation
- Individual grant QP090102
- Korea Institute for Advanced Study (KIAS)
- Individual grant CG031509
- Korea Institute for Advanced Study (KIAS)
References
Journal reference (Paper in which the method is described) W. Yang, I. Timrov, F. Aquilante, Y.-W. Son, npj Computational Materials volume 12, 323 (2026), doi: https://doi.org/10.1038/s41524-026-02123-9