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We train a neural network as the universal exchange-correlation functional of density-functional theory that simultaneously reproduces both the exact exchange-correlation energy and potential. This functional is extremely non-local, but…

Computational Physics · Physics 2019-10-10 Jonathan Schmidt , Carlos L. Benavides-Riveros , Miguel A. L. Marques

While in principle exact, Kohn-Sham density functional theory -- the workhorse of computational chemistry -- must rely on approximations for the exchange-correlation functional. Despite staggering successes, present-day approximations still…

Kohn-Sham (KS) density functional theory (DFT) is a very efficient method for calculating various properties of solids as, for instance, the total energy, the electron density, or the electronic band structure. The KS-DFT method leads to…

Materials Science · Physics 2019-09-20 Fabien Tran , Jan Doumont , Leila Kalantari , Ahmad W. Huran , Miguel A. L. Marques , Peter Blaha

Using the optimized effective potential method in conjunction with the semi-analytical approximation due to Krieger, Li and Iafrate, we have performed fully self-consistent exact exchange-only density-functional calculations for diatomic…

chem-ph · Physics 2008-02-03 T. Grabo , E. K. U. Gross

The thorough treatment of electron-lattice interactions from first principles is one of the main goals in condensed matter physics. While the commonly applied adiabatic Born-Oppenheimer approximation is sufficient for describing many…

A new method for extracting ensemble Kohn-Sham potentials from accurate excited state densities is applied to a variety of two electron systems, exploring the behavior of exact ensemble density functional theory. The issue of separating the…

A rigorous derivation of the density functional in the Hohenberg-Kohn theory is presented. With no assumption regarding the magnitude of the electric coupling constant $e^2$ (or correlation), this work provides a firm basis for…

Other Condensed Matter · Physics 2010-09-20 Yi-Kuo Yu

The uniform electron gas and the hydrogen atom play fundamental roles in condensed matter physics and quantum chemistry. The former has an infinite number of electrons uniformly distributed over the neutralizing positively-charged…

Chemical Physics · Physics 2016-06-22 Jianwei Sun , John P. Perdew , Zenghui Yang , Haowei Peng

Accurately describing excited states within Kohn-Sham (KS) density functional theory (DFT), particularly those which induce ionization and charge transfer, remains a great challenge. Common exchange-correlation (xc) approximations are…

Materials Science · Physics 2021-02-09 Eli Kraisler , M. J. P. Hodgson , E. K. U. Gross

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

Density functional theory is the workhorse of modern electronic structure calculations, with wide-ranging applications in chemistry, physics, materials science, and machine learning. At its heart lies the exchange-correlation functional, a…

Chemical Physics · Physics 2026-02-20 Fabien Tran , Susi Lehtola , Stefano Pittalis , Miguel A. L. Marques

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

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

A method for calculating the Kohn--Sham exchange-correlation potential, $v_\text{XC}(\mathbf{r})$, from a given electronic wavefunction is devised and implemented. It requires on input one- and two-electron density matrices and involves…

Chemical Physics · Physics 2015-08-19 Ilya G. Ryabinkin , Sviataslau V. Kohut , Viktor N. Staroverov

We propose a method for the evaluation of magnetic exchange couplings based on noncollinear spin-density functional calculations. The method employs the second derivative of the total Kohn-Sham energy of a single reference state, in…

Materials Science · Physics 2009-11-13 Juan E. Peralta , Veronica Barone

We construct a nonlocal density functional approximation with full exact exchange, while preserving the constraint-satisfaction approach and justified error cancellations of simpler semilocal functionals. This is achieved by interpolating…

Chemical Physics · Physics 2009-11-13 John P. Perdew , Viktor N. Staroverov , Jianmin Tao , Gustavo E. Scuseria

We obtain the exact Kohn-Sham potentials $V_{\mathrm{KS}}$ of time-dependent density-functional theory for 1D Hubbard chains, driven by a d.c.\ external field, using the time-dependent electron density and current density obtained from…

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

In this chapter, we provide a review of ground-state Kohn-Sham density-functional theory of electronic systems and some of its extensions, we present exact expressions and constraints for the exchange and correlation density functionals,…

Chemical Physics · Physics 2022-09-12 Julien Toulouse

Adiabatic time-dependent density functional theory fails for excitations of a heteroatomic molecule composed of two open-shell fragments at large separation. Strong frequency-dependence of the exchange-correlation kernel is necessary for…

Other Condensed Matter · Physics 2009-11-11 Neepa T. Maitra , David G. Tempel

Accurate treatment of the electronic correlation in inhomogeneous electronic systems, combined with the ability to capture the correlation energy of the homogeneous electron gas, allows to reach high predictive power in the application of…

Strongly Correlated Electrons · Physics 2010-06-22 E. Rasanen , S. Pittalis , C. R. Proetto
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