Iurii Timrov^1*, Nicola Marzari^1*, Matteo Cococcioni^2*

1 Theory and Simulation of Materials (THEOS), and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

2 Department of Physics, University of Pavia, via Bassi 6, I-27100 Pavia, Italy

* Corresponding authors emails: iurii.timrov@epfl.ch, nicola.marzari@epfl.ch, matteo.cococcioni@unipv.it

DOI10.24435/materialscloud:vp-wm [version v1]

Publication date: Nov 09, 2020

How to cite this record

Iurii Timrov, Nicola Marzari, Matteo Cococcioni, Self-consistent Hubbard parameters from density-functional perturbation theory in the ultrasoft and projector-augmented wave formulations, Materials Cloud Archive 2020.143 (2020), doi: 10.24435/materialscloud:vp-wm.

Description

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 LiₓMnPO₄ (x=0,1) and the subtle energetics of Li intercalation.

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Keywords

Density-functional perturbation theory Hubbard-corrected density-functional theory extended Hubbard functionals self-interaction corrections Hubbard on-site U and inter-site V parameters CSCS MARVEL ultrasoft pseudopotentials projector-augmented wave method Li-ion batteries voltages LiMnPO4 MnPO4 linear-response theory monochromatic perturbations