Self-consistent Hubbard parameters from density-functional perturbation theory in the ultrasoft and projector-augmented wave formulations

Abstract

The self-consistent evaluation of Hubbard parameters using linear-response theory is crucial for quantitatively predictive calculations based on Hubbard-corrected density-functional theory. Here, we extend a recently-introduced approach based on density-functional perturbation theory (DFPT) for the calculation of the on-site Hubbard $U$ to also compute the inter-site Hubbard $V$. DFPT allows to reduce significantly computational costs, improve numerical accuracy, and fully automate the calculation of the Hubbard parameters by recasting the linear response of a localized perturbation into an array of monochromatic perturbations that can be calculated in the primitive cell. In addition, here we generalize the entire formalism from norm-conserving to ultrasoft and projector-augmented wave formulations, and to metallic ground states. After benchmarking DFPT against the conventional real-space Hubbard linear response in a supercell, we demonstrate the effectiveness of the present extended Hubbard formulation in determining the equilibrium crystal structure of Li${}_x$MnPO${}_4$ (x=0,1) and the subtle energetics of Li intercalation.

15 pages, 3 figures

References in corpus (12)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Quantum ESPRESSO toward the exascale
• Density functional theory in transition-metal chemistry: a self-consistent Hubbard U approach
• Calculations of Hubbard U from first-principles
• Hubbard U and Hund's Exchange J in Transition Metal Oxides: Screening vs. Localization Trends from Constrained Random Phase Approximation
• Hubbard-corrected density functional perturbation theory with ultrasoft pseudopotentials
• Screened Coulomb interaction calculations: cRPA implementation and applications to dynamical screening and self-consistency in uranium dioxide and cerium
• Method for calculating the electronic structure of correlated materials from a truly first-principles LDA+U scheme
• Interplay between breathing mode distortion and magnetic order in rare-earth nickelates $R$NiO${}_3$ within DFT+$U$

Cited by in corpus (2)

• Extensive Benchmarking of DFT+U Calculations for Predicting Band Gaps
• Interaction-induced topological superconductivity in antiferromagnet-superconductor junctions