High-throughput determination of Hubbard U and Hund J values for transition metal oxides via the linear response formalism

• Published in: Physical review materials 2024-01, Vol.8 (1), Article 014409
• Main Authors: Moore, Guy C., Horton, Matthew K., Linscott, Edward, Ganose, Alexander M., Siron, Martin, O'Regan, David D., Persson, Kristin A.
• Format: Article
• Language: English
• Subjects: ab initio calculations; density functional theory; Hubbard model; MATERIALS SCIENCE
• ISSN: 2475-9953; 2475-9953
• DOI: 10.1103/PhysRevMaterials.8.014409

DFT+U provides a convenient, cost-effective correction for the self-interaction error (SIE) that arises when describing correlated electronic states using conventional approximate density functional theory (DFT). The success of a DFT+U(+J) calculation hinges on the accurate determination of its Hubbard U and Hund J parameters, and the linear response (LR) methodology has proven to be computationally effective and accurate for calculating these parameters. This study provides a high-throughput computational analysis of the U and J values for transition metal d-electron states in a representative set of over 1000 magnetic transition metal oxides (TMOs), providing a frame of reference for researchers who use DFT+U to study transition metal oxides. In order to perform this high-throughput study, an ATOMATE workflow is developed for calculating U and J values automatically on massively parallel supercomputing architectures. Here, to demonstrate an application of this workflow, the spin-canting magnetic structure and unit cell parameters of the multiferroic olivine LiNiPO4 are calculated using the computed Hubbard U and Hund J values for Ni-d and O-p states, and are compared with experiment. Both the Ni-d U and J corrections have a strong effect on the Ni-moment canting angle. Additionally, including a O-pU value results in a significantly improved agreement between the computed lattice parameters and experiment