Importance of enforcing Hund’s rules in density functional theory calculations of rare earth magnetocrystalline anisotropy
Abstract Density functional theory (DFT) and its extensions, such as DFT+U and DFT+dynamical mean-field theory, are invaluable for studying magnetic properties in solids. However, rare-earth (R) materials remain challenging due to self-interaction errors and the lack of proper orbital polarization....
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-06-01
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| Series: | npj Computational Materials |
| Online Access: | https://doi.org/10.1038/s41524-025-01632-3 |
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| author | Y. Lee Z. Ning R. Flint R. J. McQueeney I. I. Mazin Liqin Ke |
| author_facet | Y. Lee Z. Ning R. Flint R. J. McQueeney I. I. Mazin Liqin Ke |
| author_sort | Y. Lee |
| collection | DOAJ |
| description | Abstract Density functional theory (DFT) and its extensions, such as DFT+U and DFT+dynamical mean-field theory, are invaluable for studying magnetic properties in solids. However, rare-earth (R) materials remain challenging due to self-interaction errors and the lack of proper orbital polarization. We show how the orbital dependence of self-interaction error contradicts Hund’s rules and plagues magnetocrystalline anisotropy (MA) calculations, and how analyzing DFT states that respect Hund’s rules can mitigate this issue. We benchmark MA in RCo5, R 2Fe14B, and RFe12, extending prior work on RMn6Sn6, achieving excellent agreement with experiments. Additionally, we illustrate a semi-analytical perturbation approach that treats crystal fields as a perturbation in the large spin-orbit coupling limit. Using Gd-4f crystal-field splitting, this method provides a microscopic understanding of MA and enables rapid screening of high-MA materials. |
| format | Article |
| id | doaj-art-cbdcb00ecec44fb2bf7b1ec910347eac |
| institution | Kabale University |
| issn | 2057-3960 |
| language | English |
| publishDate | 2025-06-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | npj Computational Materials |
| spelling | doaj-art-cbdcb00ecec44fb2bf7b1ec910347eac2025-08-20T03:26:47ZengNature Portfolionpj Computational Materials2057-39602025-06-0111111110.1038/s41524-025-01632-3Importance of enforcing Hund’s rules in density functional theory calculations of rare earth magnetocrystalline anisotropyY. Lee0Z. Ning1R. Flint2R. J. McQueeney3I. I. Mazin4Liqin Ke5Ames National Laboratory, U.S. Department of EnergyAmes National Laboratory, U.S. Department of EnergyAmes National Laboratory, U.S. Department of EnergyAmes National Laboratory, U.S. Department of EnergyDepartment of Physics and Astronomy, George Mason UniversityAmes National Laboratory, U.S. Department of EnergyAbstract Density functional theory (DFT) and its extensions, such as DFT+U and DFT+dynamical mean-field theory, are invaluable for studying magnetic properties in solids. However, rare-earth (R) materials remain challenging due to self-interaction errors and the lack of proper orbital polarization. We show how the orbital dependence of self-interaction error contradicts Hund’s rules and plagues magnetocrystalline anisotropy (MA) calculations, and how analyzing DFT states that respect Hund’s rules can mitigate this issue. We benchmark MA in RCo5, R 2Fe14B, and RFe12, extending prior work on RMn6Sn6, achieving excellent agreement with experiments. Additionally, we illustrate a semi-analytical perturbation approach that treats crystal fields as a perturbation in the large spin-orbit coupling limit. Using Gd-4f crystal-field splitting, this method provides a microscopic understanding of MA and enables rapid screening of high-MA materials.https://doi.org/10.1038/s41524-025-01632-3 |
| spellingShingle | Y. Lee Z. Ning R. Flint R. J. McQueeney I. I. Mazin Liqin Ke Importance of enforcing Hund’s rules in density functional theory calculations of rare earth magnetocrystalline anisotropy npj Computational Materials |
| title | Importance of enforcing Hund’s rules in density functional theory calculations of rare earth magnetocrystalline anisotropy |
| title_full | Importance of enforcing Hund’s rules in density functional theory calculations of rare earth magnetocrystalline anisotropy |
| title_fullStr | Importance of enforcing Hund’s rules in density functional theory calculations of rare earth magnetocrystalline anisotropy |
| title_full_unstemmed | Importance of enforcing Hund’s rules in density functional theory calculations of rare earth magnetocrystalline anisotropy |
| title_short | Importance of enforcing Hund’s rules in density functional theory calculations of rare earth magnetocrystalline anisotropy |
| title_sort | importance of enforcing hund s rules in density functional theory calculations of rare earth magnetocrystalline anisotropy |
| url | https://doi.org/10.1038/s41524-025-01632-3 |
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