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The complex nature of electron-electron correlations is made manifest in the very simple but non-trivial problem of two electrons confined within a sphere. The description of highly non-local correlation and self-interaction effects by…

Other Condensed Matter · Physics 2016-08-16 J. Jung , P. García-González , J. E. Alvarellos , R. W. Godby

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

Self-interactions (SIs) are a major problem in density functional approximations and the source of serious divergence from experimental results. Here, we propose to optimize density functional total energies in terms of the effective local…

Other Condensed Matter · Physics 2012-06-20 Nikitas I. Gidopoulos , Nektarios N. Lathiotakis

In approximate Kohn-Sham density-functional theory, self-interaction manifests itself as the dependence of the energy of an orbital on its fractional occupation. This unphysical behavior translates into qualitative and quantitative errors…

Materials Science · Physics 2010-09-28 Ismaila Dabo , Andrea Ferretti , Nicolas Poilvert , Yanli Li , Nicola Marzari , Matteo Cococcioni

The exchange-correlation energy in Kohn-Sham density functional theory can be expressed exactly in terms of the change in the expectation of the electron-electron repulsion operator when, in the many-electron hamiltonian, this same operator…

Strongly Correlated Electrons · Physics 2009-08-05 Paola Gori-Giorgi , Giovanni Vignale , Michael Seidl

Self-interaction is a fundamental flaw of practical Kohn-Sham Density Functional Theory (KS DFT) approximations responsible for numerous qualitative and even catastrophic shortcomings. Whereas self-interaction is easy to characterize in…

Chemical Physics · Physics 2024-07-16 Samuel A. Slattery , Edward F. Valeev

We present and test a new approximation for the exchange-correlation (xc) energy of Kohn-Sham density functional theory. It combines exact exchange with a compatible non-local correlation functional. The functional is by construction free…

Chemical Physics · Physics 2014-05-23 Tobias Schmidt , Eli Kraisler , Adi Makmal , Leeor Kronik , Stephan Kümmel

The State--Specific Kohn--Sham Density Functional Theory [arXiv:physics/0506037] is used to derive the Kohn-Sham exchange-correlation potential $\vxc$ and exchange-correlation energy $\Eco$ as explicit functionals of $v_s$ and $\phi_1$,…

Chemical Physics · Physics 2025-01-31 James P. Finley

We use the exact strong-interaction limit of the Hohenberg-Kohn energy density functional to approximate the exchange-correlation energy of the restricted Kohn-Sham scheme. Our approximation corresponds to a highly non-local density…

Strongly Correlated Electrons · Physics 2012-12-12 Francesc Malet , Paola Gori-Giorgi

We introduce a new functional for simulating ground-state and time-dependent electronic systems within density-functional theory. The functional combines an expression for the exact Kohn-Sham (KS) potential in the limit of complete electron…

Mesoscale and Nanoscale Physics · Physics 2021-01-15 M. J. P. Hodgson , J. D. Ramsden , T. R. Durrant , R. W. Godby

We report on a methodology for the treatment of the Coulomb energy and potential in Kohn-Sham density functional theory that is free from self-interaction effects. Specifically, we determine the Coulomb potential given as the functional…

Materials Science · Physics 2016-06-29 M. Däne , A. Gonis , D. M. Nicholson , G. M. Stocks

Exact density functionals for the exchange and correlation energies are approximated in practical calculations for the ground-state electronic structure of a many-electron system. An important exact constraint for the construction of…

The effective potential of electron--electron interaction and the two-particle \textquotedblleft density--density\textquotedblright\ correlation function have been calculated for a simple semiinfinite metal making allowance for the…

Mesoscale and Nanoscale Physics · Physics 2015-03-29 B. M. Markovych , I. M. Zadvorniak

We present an alternative to the Kohn-Sham formulation of density functional theory for the ground-state properties of strongly interacting electronic systems. The idea is to start from the limit of zero kinetic energy and systematically…

Strongly Correlated Electrons · Physics 2015-05-13 Paola Gori-Giorgi , Michael Seidl , G. Vignale

The exchange-correlation energy in Kohn-Sham density functional theory is expressed as a functional of the electronic density and the Kohn-Sham orbitals. An alternative to Kohn-Sham theory is to express the energy as a functional of the…

Computational Physics · Physics 2009-10-31 S. Goedecker , C. Umrigar

Ground and excited states of a confined negative Hydrogen ion has been pursued under Kohn-Sham density functional approach by invoking a physically motivated work-function-based exchange potential. The exchange-only results are of near…

Atomic Physics · Physics 2022-05-23 Sangita Majumdar , Neetik Mukherjee , Amlan K. Roy

By propagating the many-body Schr\"odinger equation, we determine the exact time-dependent Kohn-Sham potential for a system of strongly correlated electrons which undergo field-induced tunneling. Numerous features are entirely absent from…

Strongly Correlated Electrons · Physics 2021-01-15 Matthew J. P. Hodgson , James D. Ramsden , Jacob B. J. Chapman , Piers Lillystone , Rex W Godby

A generalization of the Kohn--Sham approach is derived where the correlation-energy functional depends on the one-particle density matrix of noninteracting states and on the external potential from the interacting target-state. The…

Chemical Physics · Physics 2007-05-23 James P. Finley

We discuss energy densities in the strong-interaction limit of density functional theory, deriving an exact expression within the definition (gauge) of the electrostatic potential of the exchange-correlation hole. Exact results for small…

Chemical Physics · Physics 2012-11-14 André Mirtschink , Michael Seidl , Paola Gori-Giorgi

In the exact Kohn-Sham density-functional theory (DFT), the total energy versus the number of electrons is a series of linear segments between integer points. However, commonly used approximate density functionals produce total energies…

Materials Science · Physics 2013-04-03 Eli Kraisler , Leeor Kronik
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