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

Abstract

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 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.

18 pages, 6 figures

References in corpus (13)

• Array Programming with NumPy
• Strong electronic correlations from Hund's coupling
• Density functional theory in transition-metal chemistry: a self-consistent Hubbard U approach
• Hubbard U and Hund's Exchange J in Transition Metal Oxides: Screening vs. Localization Trends from Constrained Random Phase Approximation
• Orbital Graph Convolutional Neural Network for Material Property Prediction
• Noncollinear Magnetism in Density Functional Calculations
• Recovering the flat-plane condition in electronic structure theory at semi-local DFT cost
• Field-induced magnetic phases and electric polarization in LiNiPO4
• DFT+U+J with linear response parameters predicts non-magnetic oxide band gaps with hybrid-functional accuracy
• Dzyaloshinskii-Moriya interaction and the magnetic ground state in magnetoelectric LiCoPO${}_4$
• A DFT+U type functional derived to explicitly address the flat plane condition
• Combining electronic structure and many-body theory with large data-bases: a method for predicting the nature of 4f states in Ce compounds
• Noncollinear DFT+$U$ and Hubbard parameters with fully-relativistic ultrasoft pseudopotentials

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