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’s 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 2000 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 LiNiPO 4 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.

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