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  4. koopmans: An Open-Source Package for Accurately and Efficiently Predicting Spectral Properties with Koopmans Functionals
 
research article

koopmans: An Open-Source Package for Accurately and Efficiently Predicting Spectral Properties with Koopmans Functionals

Linscott, Edward Baxter  
•
Colonna, Nicola  
•
De Gennaro, Riccardo  
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August 23, 2023
Journal of Chemical Theory and Computation

Over the past decade we have developed Koopmans functionals, a computationally efficient approach for predicting spectral properties with an orbital-density-dependent functional framework. These functionals impose a generalized piecewise linearity condition to the entire electronic manifold, ensuring that orbital energies match the corresponding electron removal/addition energy differences (in contrast to semilocal DFT, where a mismatch between the two lies at the heart of the band gap problem and, more generally, the unreliability of Kohn-Sham orbital energies). This strategy has proven to be very powerful, yielding molecular orbital energies and solid-state band structures with comparable accuracy to many-body perturbation theory but at greatly reduced computational cost while preserving a functional formulation. This paper reviews the theory of Koopmans functionals, discusses the algorithms necessary for their implementation, and introduces koopmans, an open-source package that contains all of the code and workflows needed to perform Koopmans functional calculations and obtain reliable spectral properties of molecules and materials.

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Type
research article
DOI
10.1021/acs.jctc.3c00652
Web of Science ID

WOS:001114702100001

Author(s)
Linscott, Edward Baxter  
Colonna, Nicola  
De Gennaro, Riccardo  
Nguyen, Ngoc Linh
Borghi, Giovanni  
Ferretti, Andrea
Dabo, Ismaila
Marzari, Nicola  
Date Issued

2023-08-23

Publisher

Amer Chemical Soc

Published in
Journal of Chemical Theory and Computation
Subjects

Physical Sciences

•

Self-Interaction Correction

•

Electron Correlation

•

Exact Exchange

•

Hartree-Fock

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Ab-Initio

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Photoelectron

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Densities

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States

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Spectroscopy

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Insulators

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
THEOS  
FunderGrant Number

Division of Materials Research

179138

Swiss National Science Foundation

205602

NCCR MARVEL, a National Centre of Competence in Research - Swiss National Science Foundation

HORIZON-EUROHPC-JU-2021-COE-01

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Available on Infoscience
February 20, 2024
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/204510
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