Comparing Hubbard parameters from linear-response theory and Hartree-Fock-based approach
Fuente:
arXiv
Gespeichert in:
| Hauptverfasser: | , , , |
|---|---|
| Format: | Preprint |
| Veröffentlicht: |
2025
|
| Schlagworte: | |
| Online-Zugang: | |
| Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
| _version_ | 1866915689819799552 |
|---|---|
| author | Yang, Wooil Timrov, Iurii Aquilante, Francesco Son, Young-Woo |
| author_facet | Yang, Wooil Timrov, Iurii Aquilante, Francesco Son, Young-Woo |
| contents | Density-functional theory with on-site $U$ and inter-site $V$ Hubbard corrections (DFT+$U$+$V$) is a powerful and accurate method for predicting various properties of transition-metal compounds. However, its accuracy depends critically on the values of these Hubbard parameters. Although they can be determined empirically, first-principles methods provide a more consistent and reliable approach; yet, their results can vary, and a comprehensive comparison between methods is still lacking. Here, we present a systematic comparison of two widely used approaches for computing $U$ and $V$, namely linear-response theory (LRT) and the Hartree-Fock-based pseudohybrid functional formalism, applied to a representative set of oxides (MnO, NiO, CoO, FeO, BaTiO$_3$, ZnO, and ZrO$_2$). We find that for partially occupied transition-metal $d$ states, these two methods yield consistent $U$ values, but they differ for nearly empty or fully filled $d$ shells. For O-$2p$ states, LRT always predicts large $U$ values ($\sim$10 eV), whereas the pseudohybrid formalism produces system-dependent values depending on the level of localization and hybridization for the electronic states. Even larger differences are found for the inter-site $V$: the former predicts consistently small values ($<1$ eV), while the latter produces larger values ($\sim3$ eV), reflecting its explicit dependence on relative charge redistribution. Our results show that while parallels between these two methods exist, they rely on distinct assumptions for determining $U$ and $V$, leading to variations in predictions of material properties. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2512_16803 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Comparing Hubbard parameters from linear-response theory and Hartree-Fock-based approach Yang, Wooil Timrov, Iurii Aquilante, Francesco Son, Young-Woo Materials Science Density-functional theory with on-site $U$ and inter-site $V$ Hubbard corrections (DFT+$U$+$V$) is a powerful and accurate method for predicting various properties of transition-metal compounds. However, its accuracy depends critically on the values of these Hubbard parameters. Although they can be determined empirically, first-principles methods provide a more consistent and reliable approach; yet, their results can vary, and a comprehensive comparison between methods is still lacking. Here, we present a systematic comparison of two widely used approaches for computing $U$ and $V$, namely linear-response theory (LRT) and the Hartree-Fock-based pseudohybrid functional formalism, applied to a representative set of oxides (MnO, NiO, CoO, FeO, BaTiO$_3$, ZnO, and ZrO$_2$). We find that for partially occupied transition-metal $d$ states, these two methods yield consistent $U$ values, but they differ for nearly empty or fully filled $d$ shells. For O-$2p$ states, LRT always predicts large $U$ values ($\sim$10 eV), whereas the pseudohybrid formalism produces system-dependent values depending on the level of localization and hybridization for the electronic states. Even larger differences are found for the inter-site $V$: the former predicts consistently small values ($<1$ eV), while the latter produces larger values ($\sim3$ eV), reflecting its explicit dependence on relative charge redistribution. Our results show that while parallels between these two methods exist, they rely on distinct assumptions for determining $U$ and $V$, leading to variations in predictions of material properties. |
| title | Comparing Hubbard parameters from linear-response theory and Hartree-Fock-based approach |
| topic | Materials Science |
| url | https://arxiv.org/abs/2512.16803 |