High-throughput determination of Hubbard U and Hund J values for transition metal oxides via the linear response formalism
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. 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 -p U value results in a significantly improved agreement between the computed lattice parameters and experiment.
WOS:001157083000004
2024-01-29
8
1
014409
REVIEWED
Funder | Grant Number |
Department of Energy Computational Science Graduate Fellowship (DOE CSGF) | DE-SC0020347 |
Swiss National Science Foundation (SNSF) | 200021-179138 |
Science Foundation Ireland (SFI) | 19/EPSRC/3605 |
Engineering and Physical Sciences Research Council | EP/S030263/1 |
European Regional Development Fund under the SFI AMBER award | |
National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility | DE-AC02- 05CH11231 |
U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division | DE-AC02-05CH11231 |