Importance of enforcing Hund’s rules in density functional theory calculations of rare earth magnetocrystalline anisotropy

Lee, Y.; Ning, Z.; Flint, R.; McQueeney, R. J.; Mazin, I. I.; Ke, Liqin

doi:10.1038/s41524-025-01632-3

Importance of enforcing Hund’s rules in density functional theory calculations of rare earth magnetocrystalline anisotropy

Journal Article · Wed Jun 04 20:00:00 EDT 2025 · npj Computational Materials

DOI:https://doi.org/10.1038/s41524-025-01632-3· OSTI ID:2571569

Lee, Y. ^[1]; ^[1]; Flint, R. ^[2]; McQueeney, R. J. ^[2]; ^[3]; ^[1]

Ames Laboratory (AMES), Ames, IA (United States)
Ames Lab., and Iowa State Univ., Ames, IA (United States)
George Mason Univ., Fairfax, VA (United States)

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, R₂Fe₁₄B, 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.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); National Science Foundation (NSF)

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 2571569

Journal Information:: npj Computational Materials, Journal Name: npj Computational Materials Journal Issue: 1 Vol. 11; ISSN 2057-3960

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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