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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

The ground state of atoms from H to Ar was calculated using a self-interaction correction to local and gradient dependent density functionals. The correction can significantly improve the total energy and makes the orbital energies…

Atomic and Molecular Clusters · Physics 2013-08-29 Simon Klüpfel , Peter Klüpfel , Hannes Jonsson

Coulomb interactions that occur in electronic structure calculations are correlated by allowing basis function components of the interacting densities to polarize, thereby reducing the magnitude of the interaction. Exchange integrals of…

Chemical Physics · Physics 2022-05-16 Jerry L. Whitten

Various orbital-dependent exchange-only potentials are studied which exhibit correct long-range asymptotic behaviour. We present the first application of these potentials for polymers and by one of these potentials for molecules. Kohn-Sham…

Condensed Matter · Physics 2007-05-23 P. S"ule , S. Kurth , V. Van Doren

We present a generalized formulation of the Optimized Effective Potential (OEP) approach to the Self Interaction Correction (SIC) problem in Time Dependent (TD) Density Functional Theory (DFT). The formulation relies on the introduction of…

Quantum Physics · Physics 2016-02-03 J. Messud , P. M. Dinh , P. -G. Reinhard , E. ~Suraud

The random phase approximation (RPA) for the electron correlation energy, combined with the exact-exchange energy, represents the state-of-the-art exchange-correlation functional within density-functional theory (DFT). However, the standard…

Other Condensed Matter · Physics 2015-05-20 Xinguo Ren , Patrick Rinke , Alexandre Tkatchenko , Matthias Scheffler

Semilocal density-functional approximations (DFAs), including the state-of-the-art SCAN functional, are plagued by the self-interaction error (SIE). While this error is explicitly defined only for one-electron systems, it has inspired the…

Materials Science · Physics 2024-01-23 Sheng Bi , Christian Carbogno , Igor Ying Zhang , Matthias Scheffler

Local-spin-density functional calculations may be affected by severe errors when applied to the study of magnetic and strongly-correlated materials. Some of these faults can be traced back to the presence of the spurious self-interaction in…

Materials Science · Physics 2009-11-10 Alessio Filippetti , Nicola Spaldin

In the constrained minimization method of Gidopoulos and Lathiotakis (J. Chem. Phys. 136, 224109), the Hartree exchange and correlation Kohn-Sham potential of a finite $N$-electron system is replaced by the electrostatic potential of an…

Chemical Physics · Physics 2018-08-01 Tom Pitts , Nikitas I. Gidopoulos , Nektarios N. Lathiotakis

The large-$Z$ asymptotic expansion of atomic energies has been useful in determining exact conditions for corrections to the local density approximation in density functional theory. The correction for exchange is fit well with a leading $Z…

Chemical Physics · Physics 2023-04-13 Nathan Argaman , Jeremy Redd , Antonio C. Cancio , Kieron Burke

The combination of density functional theory with other approaches to the many-electron problem through the separation of the electron-electron interaction into a short-range and a long-range contribution is a promising method, which is…

Materials Science · Physics 2009-11-11 Paola Gori-Giorgi , Andreas Savin

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

We propose approximations which go beyond the local density approximation for the short-range exchange and correlation density functionals appearing in a multi-determinantal extension of the Kohn-Sham scheme. A first approximation consists…

Chemical Physics · Physics 2009-11-10 Julien Toulouse , Francois Colonna , Andreas Savin

We generalize the exact strong-interaction limit of the exchange-correlation energy of Kohn-Sham density functional theory to open systems with fluctuating particle numbers. When used in the self-consistent Kohn-Sham procedure on…

Strongly Correlated Electrons · Physics 2015-06-16 André Mirtschink , Michael Seidl , Paola Gori-Giorgi

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 exact exchange potential in time-dependent density-functional theory is defined as an orbital functional through the time-dependent optimized effective potential (TDOEP) method. We numerically solve the TDOEP integral equation for the…

Mesoscale and Nanoscale Physics · Physics 2009-11-13 H. O. Wijewardane , C. A. Ullrich

Using an end-to-end differentiable implementation of the Kohn-Sham self-consistent field equations, we obtain an accurate neural network-based exchange and correlation (XC) functional of the electronic density. The functional is optimized…

Chemical Physics · Physics 2021-06-09 Sebastian Dick , Marivi Fernandez-Serra

The derivative discontinuity of the exchange-correlation functional of density-functional theory is cast as the difference of two types of electron affinities. We show that standard Kohn-Sham calculations can be used to calculate both…

Chemical Physics · Physics 2007-12-13 F. P. Rosselli , A. B. F. da Silva , K. Capelle

The conventional approaches to the inverse density functional theory problem typically assume non-degeneracy of the Kohn-Sham (KS) eigenvalues, greatly hindering their use in open-shell systems. We present a generalization of the inverse…

Chemical Physics · Physics 2024-01-09 Bikash Kanungo , Jeffrey Hatch , Paul M. Zimmerman , Vikram Gavini

For a three-electron system with finite-strength interactions confined to a one-dimensional harmonic trap, we solve the Schroedinger equation analytically to obtain the exact solutions, from which we construct explicitly the simultaneous…

Mesoscale and Nanoscale Physics · Physics 2018-11-14 Taichi Kosugi , Yu-ichiro Matsushita
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