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research article

Koopmans Spectral Functionals in Periodic Boundary Conditions

Colonna, Nicola  
•
De Gennaro, Riccardo  
•
Linscott, Edward  
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August 4, 2022
Journal of Chemical Theory and Computation

Koopmans spectral functionals aim to describe simultaneously ground-state properties and charged excitations of atoms, molecules, nanostructures, and periodic crystals. This is achieved by augmenting standard density functionals with simple but physically motivated orbital-density-dependent corrections. These corrections act on a set of localized orbitals that, in periodic systems, resemble maximally localized Wannier functions. At variance with the original, direct supercell implementation (Phys. Rev. X 2018, 8, 021051), we discuss here (i) the complex but efficient formalism required for a periodic boundary code using explicit Brillouin zone sampling and (ii) the calculation of the screened Koopmans corrections with density functional perturbation theory. In addition to delivering improved scaling with system size, the present development makes the calculation of band structures with Koopmans functionals straightforward. The implementation in the open-source Quantum ESPRESSO distribution and the application to prototypical insulating and semiconducting systems are presented and discussed.

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Type
research article
DOI
10.1021/acs.jctc.2c00161
Web of Science ID

WOS:000837849300001

Author(s)
Colonna, Nicola  
De Gennaro, Riccardo  
Linscott, Edward  
Marzari, Nicola  
Date Issued

2022-08-04

Publisher

AMER CHEMICAL SOC

Published in
Journal of Chemical Theory and Computation
Subjects

Chemistry, Physical

•

Physics, Atomic, Molecular & Chemical

•

Chemistry

•

Physics

•

self-interaction correction

•

greens-function

•

ab-initio

•

electronic-structure

•

orbital energies

•

hartree-fock

•

density

•

exchange

•

states

•

charge

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
THEOS  
Available on Infoscience
August 29, 2022
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/190327
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