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Despite the success of density functional approximations (DFAs) in describing the electronic properties of many-electron systems, the most widely used approximations suffer from self-interaction errors (SIE) that limit their predictive…

Chemical Physics · Physics 2020-01-08 Yoh Yamamoto , Carlos M. Diaz , Luis Basurto , Koblar A. Jackson , Tunna Baruah , Rajendra R. Zope

Recently developed locally scaled self-interaction correction (LSIC) is a one-electron SIC method that, when used with a ratio of kinetic energy densities (z$_\sigma$) as iso-orbital indicator, performs remarkably well for both…

Chemical Physics · Physics 2024-01-31 Rajendra R. Zope , Yoh Yamamoto , Tunna Baruah

We investigate from a practitioner's point of view the computation of the ionization potential (IP) within density functional theory (DFT). DFT with (semi-)local energy-density functionals is plagued by a self-interaction error which…

Atomic and Molecular Clusters · Physics 2015-06-16 Peter Klüpfel , Mai Phuong Dinh , Paul-Gerhard Reinhard , Eric Suraud

The Perdew-Zunger (PZ) self-interaction correction (SIC) is an established tool to correct unphysical behavior in density functional approximations. Yet, PZ-SIC is well-known to sometimes break molecular symmetries. An example of this is…

Chemical Physics · Physics 2024-10-28 Sebastian Schwalbe , Wanja Timm Schulze , Kai Trepte , Susi Lehtola

Accurate prediction of spin-state energy difference is crucial for understanding the spin crossover (SCO) phenomena and is very challenging for the density functional approximations, especially for the local and semi-local approximations,…

Chemical Physics · Physics 2023-02-22 Selim Romero , Tunna Baruah , Rajendra R. Zope

The Fermi-L\"owdin orbital (FLO) approach to the Perdew-Zunger self-interaction correction (PZ-SIC) to density functional theory (DFT) is described and an improved approach to the problem of optimizing the Fermi-orbitals in order to…

Chemical Physics · Physics 2019-10-24 K. A. Jackson , J. E. Peralta , R. P. Joshi , K. P. Withanage , K. Trepte , K. Sharkas , A. I. Johnson

Self-interaction error (SIE), arising from the imperfect cancellation of the spurious classical Coulomb interaction between an electron and itself, is a persistent challenge in modern density functional approximations. This issue is…

It is demonstrated that the commonly applied self interaction correction (SIC) used in density functional theory does not remove all self interaction. We present as an alternative a novel method which, by construction, is totally free from…

Materials Science · Physics 2007-05-23 Urban Lundin , Olle Eriksson

(Semi)-local density functional approximations (DFAs) suffer from self-interaction error (SIE). When the first ionization energy (IE) is computed as the negative of the highest-occupied orbital (HO) eigenvalue, DFAs notoriously…

Perdew-Zunger self-interaction correction (PZ-SIC) offers a route to remove self-interaction errors on an orbital-by-orbital basis. A recent formulation of PZ-SIC by Pederson, Ruzsinszky and Perdew proposes restricting the unitary…

Chemical Physics · Physics 2021-12-07 Carlos M. Diaz , Tunna Baruah , Rajendra R. Zope

Qualitatively incorrect results are obtained for the Mn dimer in density functional theory calculations using the generalized gradient approximation (GGA) and similar results are obtained from local density and meta-GGA functionals. The…

Chemical Physics · Physics 2021-05-18 Aleksei V. Ivanov , Tushar K. Ghosh , Elvar Ö. Jónsson , Hannes Jónsson

We study the effect of self-interaction errors on the barrier heights of chemical reactions. For this purpose we use the well-known Perdew-Zunger [J. P. Perdew and A. Zunger, Phys. Rev. B, {\bf 23}, 5048 (1981)] self-interaction-correction…

The Strongly Constrained and Appropriately Normed (SCAN) functional is a non-empirical meta-generalized-gradient approximation (meta-GGA) functional that satisfies all the known constraints that a meta-GGA functional can, but it also…

Materials Science · Physics 2020-04-29 Yoh Yamamoto , Alan Salcedo , Carlos M. Diaz , Md Shamsul Alam , Tunna Baruah , Rajendra R. Zope

Density functional approximations are known to significantly overestimate the polarizabilities of long chain-like molecules. We study the static electric dipole polarizabilities and the vertical ionization potentials of polyacenes from…

Chemical Physics · Physics 2021-03-10 Sharmin Akter , Yoh Yamamoto , Rajendra R. Zope , Tunna Baruah

The Perdew-Zunger self-interaction correction cures many common problems associated with semilocal density functionals, but suffers from a size-extensivity problem when Kohn-Sham orbitals are used in the correction. Fermi-L\"{o}wdin-orbital…

Computational Physics · Physics 2017-06-30 Zeng-hui Yang , Mark R. Pederson , John P. Perdew

We calculate the electronic structure of several atoms and small molecules by direct minimization of the Self-Interaction Corrected Local Density Approximation (SIC-LDA) functional. To do this we first derive an expression for the gradient…

Condensed Matter · Physics 2009-10-28 S. Goedecker , C. J. Umrigar

In effective single-electron theories, self-interaction manifests itself through the unphysical dependence of the energy of an electronic state as a function of its occupation, which results in important deviations from the ideal Koopmans…

Materials Science · Physics 2009-01-20 I. Dabo , M. Cococcioni , N. Marzari

The most widely-used density functionals for the exchange-correlation energy are inexact for one-electron systems. Their self-interaction errors can be severe in some applications. The problem is not only to correct the self-interaction…

Chemical Physics · Physics 2009-11-10 Stephan Kümmel , John P. Perdew

We find that for simple metal clusters a single-electron description of the ground state employing self-interaction correction (SIC) in the framework of local-density approximation strongly contaminates the high energy photoionization cross…

Atomic and Molecular Clusters · Physics 2009-11-07 M. E. Madjet , Himadri S. Chakraborty , Jan-M. Rost

A systematic comparison of three approximate self-interaction corrections (SICs), Perdew-Zunger SIC, Lundin-Eriksson SIC and extended Fermi-Amaldi SIC, is performed for a model Hamiltonian whose exact many-body solution and exact…

Materials Science · Physics 2008-07-18 Daniel Vieira , K. Capelle