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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

We propose a novel scheme to bring reduced density matrix functional theory (RDMFT) into the realm of density functional theory (DFT) that preserves the accurate density functional description at equilibrium, while incorporating accurately…

Chemical Physics · Physics 2014-11-07 Nektarios N. Lathiotakis , Nicole Helbig , Angel Rubio , Nikitas I. Gidopoulos

We prove that the electron density function of a real physical system can be uniquely determined by its values on any finite subsystem. This establishes the existence of a rigorous density-functional theory for any open electronic system.…

Quantum Physics · Physics 2007-05-23 Xiao Zheng , Fan Wang , GuanHua Chen

Gould and Pittalis [Phys. Rev. Lett. 123, 016401 (2019)] recently revealed a density-driven (DD) correlation energy that is specific to many-electron ensembles and must be accounted for by approximations. We derive in this Letter a general…

Chemical Physics · Physics 2020-06-22 Emmanuel Fromager

Kohn-Sham density functional theory (KS-DFT) has found widespread application in accurate electronic structure calculations. However, it can be computationally demanding especially for large-scale simulations, motivating recent efforts…

Computational Physics · Physics 2024-06-25 Feitong Song , Ji Feng

Typical density functional theory (DFT) and approximations thereto solve the many-electron ground state problem by working from a numerically efficient non-interacting Kohn-Sham reference system; and benefit from useful minimization…

Chemical Physics · Physics 2025-04-02 Tim Gould

Density functional theory (DFT) and beyond-DFT methods are often used in combination with photoelectron spectroscopy to obtain physical insights into the electronic structure of molecules and solids. The Kohn-Sham eigenvalues are not…

An accurate expression of the kinetic energy density of an electronic distribution in terms of the single particle reduced density matrix for atomic and molecular systems is a long-standing problem in electron structure theory. Existing…

Chemical Physics · Physics 2024-10-30 Priya , Mainak Sadhukhan

This is a comprehensive review of the strong-interaction limit of density functional theory. It covers the derivation of the limiting strictly correlated electrons (SCE) functional from exact Hohenberg-Kohn DFT, basic aspects of SCE physics…

Chemical Physics · Physics 2022-02-22 Gero Friesecke , Augusto Gerolin , Paola Gori-Giorgi

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

Accurate first-principles calculations for the energies, charge distributions, and spin symmetries of many-electron systems are essential to understand and predict the electronic and structural properties of molecules and materials.…

Chemical Physics · Physics 2024-01-24 Yuming Shi , Yi Shi , Adam Wasserman

The description of interacting many-electron systems in external magnetic fields is considered in the framework of the optimized effective potential method extended to current-spin-density functional theory. As a case study, a…

Materials Science · Physics 2011-01-14 N. Helbig , S. Kurth , S. Pittalis , E. Räsänen , E. K. U. Gross

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

A new formalism to describe steady-state electronic and thermal transport in the framework of density functional theory is presented. A one-to-one correspondence is proven between the three basic variables of the theory, i.e., the density…

Mesoscale and Nanoscale Physics · Physics 2022-04-26 Nahual Sobrino , Florian Eich , Gianluca Stefanucci , Roberto D'Agosta , Stefan Kurth

In the density functional (DF) theory of Kohn and Sham, the kinetic energy of the ground state of a system of noninteracting electrons in a general external field is calculated using a set of orbitals. Orbital free methods attempt to…

Strongly Correlated Electrons · Physics 2009-11-13 Jeng-Da Chai , John D Weeks

We consider density functionals for exchange and correlation energies in two-dimensional systems. The functionals are constructed by making use of exact constraints for the angular averages of the corresponding exchange and correlation…

Strongly Correlated Electrons · Physics 2010-02-25 E. Rasanen , S. Pittalis

Kohn-Sham density functional theory is one of the most widely used electronic structure theories. In the pseudopotential framework, uniform discretization of the Kohn-Sham Hamiltonian generally results in a large number of basis functions…

Numerical Analysis · Mathematics 2015-05-27 Lin Lin , Jianfeng Lu , Lexing Ying , E. Weinan

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

In spin-density-functional theory for noncollinear magnetic materials, the Kohn-Sham system features exchange-correlation (xc) scalar potentials and magnetic fields. The significance of the xc magnetic fields is not very well explored; in…

Materials Science · Physics 2019-09-25 Edward A. Pluhar , Carsten A. Ullrich

A rigorous derivation of the density functional via the effective action in the Hohenberg-Kohn theory is outlined. Using the auxiliary field method, in which the electric coupling constant $e^2$ need not be small, we show that the loop…

Other Condensed Matter · Physics 2009-09-22 Yi-Kuo Yu