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We present a new density-functional method of the self-consistent electronic-structure calculation which does not exploit any local density approximations (LDA). We use the exchange-correlation energy which consists of the exact exchange…

Statistical Mechanics · Physics 2009-10-30 Takao Kotani

Over the past few years it has been pointed out that direct inversion of accurate but approximate ground state densities leads to Kohn-Sham exchange-correlation (xc) potentials that can differ significantly from the exact xc potential of a…

Atomic Physics · Physics 2020-08-26 Ashish Kumar , Rabeet Singh , Manoj K. Harbola

Ground-state Kohn-Sham density functional theory provides, in principle, the exact ground-state energy and electronic spin-densities of real interacting electrons in a static external potential. In practice, the exact density functional for…

Chemical Physics · Physics 2022-07-11 Aaron D. Kaplan , Mel Levy , John P. Perdew

We construct exact Kohn-Sham potentials for the ensemble density-functional theory (EDFT) from the ground and excited states of helium. The exchange-correlation (XC) potential is compared with the quasi-local-density approximation and both…

A direct orbital optimization method is presented for density functional calculations of excited electronic states using either a real space grid or a plane wave basis set. The method is variational, provides atomic forces in the excited…

Computational Physics · Physics 2022-11-09 Aleksei V. Ivanov , Gianluca Levi , Elvar Ö. Jónsson , Hannes Jónsson

In the search for an accurate and computationally efficient approximation to the exact exchange potential of Kohn-Sham density functional theory, we recently compared various semilocal exchange potentials to the exact one [F. Tran et al.,…

Strongly Correlated Electrons · Physics 2016-10-21 Fabien Tran , Peter Blaha , Markus Betzinger , Stefan Blügel

We develop a novel approach to the coupled motion of electrons and ions that focuses on the dynamics of the electronic subsystem. Usually the description of electron dynamics involves an electronic Schr\"odinger equation where the nuclear…

Chemical Physics · Physics 2013-11-18 Yasumitsu Suzuki , Ali Abedi , Neepa T. Maitra , Koichi Yamashita , E. K. U. Gross

We model the Hartree-exchange-correlation potential of Kohn-Sham density-functional theory adopting a novel strategy inspired by the strictly-correlated-electrons limit and relying on the exact decomposition of the potential based on the…

Chemical Physics · Physics 2024-09-09 Sara Giarrusso , Federica Agostini

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

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

We present an implementation of the optimised effective potential (OEP) scheme for the exact-exchange (EXX) and random phase approximation (RPA) energy functionals and apply these methods to a range of bulk materials. We calculate the…

Materials Science · Physics 2014-05-16 Jiří Klimeš , Georg Kresse

If one-electron observables of a many-electron system are of interest, a many-electron dynamics can be represented exactly by a one-electron dynamics with effective potentials. The formalism for this reduction is provided by the Exact…

Chemical Physics · Physics 2021-01-04 Jakub Kocák , Axel Schild

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

We present an efficient method for propagating the time-dependent Kohn-Sham equations in free space, based on the recently introduced Fourier contour deformation (FCD) approach. For potentials which are constant outside a bounded domain,…

Chemical Physics · Physics 2023-07-10 Jason Kaye , Alex Barnett , Leslie Greengard , Umberto De Giovannini , Angel Rubio

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 Hartree-Fock exchange operator is an integral operator arising in the Hartree-Fock method and replaced by a multiplicative operator (a local potential) in Kohn-Sham density functional theory. This article presents a detailed analysis of…

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

In electronic structure calculations the optimized effective potential (OEP) is a method that treats exchange interactions exactly using a local potential within density-functional theory (DFT). We present a method using density functional…

Materials Science · Physics 2013-01-24 Tom W. Hollins , Stewart J. Clark , Keith Refson , Nikitas I. Gidopoulos

The optimized effective potential method is formulated as a convex minimization problem. This formulation does not require assumptions about $v$-representability nor functional differentiability. The formulation provides a natural framework…

Chemical Physics · Physics 2022-02-01 Erik I. Tellgren , Andre Laestadius , Markus Penz

We consider an optimal control problem constrained by a parabolic partial differential equation (PDE) with Robin boundary conditions. We use a well-posed space-time variational formulation in Lebesgue--Bochner spaces with minimal…

Numerical Analysis · Mathematics 2022-12-06 Nina Beranek , M. Alexander Reinhold , Karsten Urban