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research article

Hubbard-corrected density functional perturbation theory with ultrasoft pseudopotentials

Floris, A.
•
Timrov, I
•
Himmetoglu, B.
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February 19, 2020
Physical Review B

We present in full detail a newly developed formalism enabling density functional perturbation theory (DFPT) calculations from a DFT + U ground state. The implementation includes ultrasoft pseudopotentials and is valid for both insulating and metallic systems. It aims at fully exploiting the versatility of DFPT combined with the low-cost DFT + U functional. This allows us to avoid computationally intensive frozen-phonon calculations when DFT + U is used to eliminate the residual electronic self-interaction from approximate functionals and to capture the localization of valence electrons, e.g., on d or f states. In this way, the effects of electronic localization (possibly due to correlations) are consistently taken into account in the calculation of specific phonon modes, Born effective charges, dielectric tensors, and in quantities requiring well converged sums over many phonon frequencies, as phonon density of states and free energies. The new computational tool is applied to two representative systems, namely CoO, a prototypical transition metal monoxide and LiCoO2, a material employed for the cathode of Li-ion batteries. The results show the effectiveness of our formalism to capture in a quantitatively reliable way the vibrational properties of systems with localized valence electrons.

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Type
research article
DOI
10.1103/PhysRevB.101.064305
Web of Science ID

WOS:000514315100003

Author(s)
Floris, A.
Timrov, I
Himmetoglu, B.
Marzari, N.  
de Gironcoli, S.
Cococcioni, M.
Date Issued

2020-02-19

Publisher

AMER PHYSICAL SOC

Published in
Physical Review B
Volume

101

Issue

6

Article Number

064305

Subjects

Materials Science, Multidisciplinary

•

Physics, Applied

•

Physics, Condensed Matter

•

Materials Science

•

Physics

•

fractionally occupied states

•

self-interaction correction

•

lithium-ion batteries

•

ab-initio calculation

•

electronic-structure

•

thermodynamic properties

•

phonon dispersions

•

lattice-dynamics

•

cobalt oxide

•

licoo2

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
THEOS  
Available on Infoscience
March 5, 2020
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/167013
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