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A long-standing puzzle in density-functional theory is the issue of the long-range behavior of the Kohn-Sham exchange-correlation potential at metal surfaces. As an important step towards its solution, it is proved here, through a rigurouos…

Materials Science · Physics 2015-05-18 C. M. Horowitz , C. R. Proetto , J. M. Pitarke

Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…

Chemical Physics · Physics 2015-06-12 Jason D. Goodpaster , Taylor A. Barnes , Frederick R. Manby , Thomas F. Miller

As a proof of principle, self-consistent Kohn--Sham calculations are performed with the exact exchange-correlation functional. Finding the exact functional for even one trial density requires solving the interacting Schr\"odinger equation…

Chemical Physics · Physics 2014-07-14 Lucas O. Wagner , Thomas E. Baker , E. M. Stoudenmire , Kieron Burke , Steven R. White

The electronic and magnetic properties of many strongly-correlated systems are controlled by a limited number of states, located near the Fermi level and well isolated from the rest of the spectrum. This opens a formal way for combining the…

Strongly Correlated Electrons · Physics 2010-07-15 I. V. Solovyev

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

Kohn-Sham density functional theory (DFT) is the workhorse of quantum chemistry, offering an attractive balance between accuracy and computational cost. Although exact in principle, DFT in practice relies on an approximation to the unknown…

Quantum Physics · Physics 2026-05-12 Karim K. Alaa El-Din , Antonius v. Strachwitz , Sam M. Vinko

We propose a machine learning based approach to develop the exchange-correlation potential of time dependent density functional theory (TDDFT). The neural network projection from the time-varying electron densities to the corresponding…

Computational Physics · Physics 2020-05-20 Yasumitsu Suzuki , Ryo Nagai , Jun Haruyama

Modern density functional theory (DFT) calculations employ the Kohn-Sham (KS) system of non-interacting electrons as a reference, with all complications buried in the exchange-correlation energy (Exc). The adiabatic connection formula gives…

Other Condensed Matter · Physics 2009-10-02 Zhenfei Liu , Kieron Burke

The behavior of the surface barrier that forms at the metal-vacuum interface is important for several fields of surface science. Within the Density Functional Theory framework, this surface barrier has two non-trivial components: exchange…

Other Condensed Matter · Physics 2009-11-11 C. M. Horowitz , C. R. Proetto , S. Rigamonti

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

The properties of the Kohn-Sham (KS) exchange potential for open systems in thermodynamical equilibrium, where the number of particles is non-conserved, are analyzed with the Optimized Effective Potential (OEP) method of Density Functional…

Other Condensed Matter · Physics 2015-06-25 S. Rigamonti , C. R. Proetto , F. A. Reboredo

When running time-dependent density functional theory (TDDFT) calculations for real-time simulations of non-equilibrium dynamics, the user has a choice of initial Kohn-Sham state, and typically a Slater determinant is used. We explore the…

Chemical Physics · Physics 2016-08-24 Johanna I. Fuks , Soeren E. B. Nielsen , Michael Ruggenthaler , Neepa T. Maitra

Kohn-Sham density functional theory (DFT) has become established as an indispensable tool for investigating aqueous systems of all kinds, including those important in chemistry, surface science, biology and the earth sciences. Nevertheless,…

Materials Science · Physics 2016-05-04 M. J. Gillan , D. Alfè , A. Michaelides

Time-dependent (current) density functional theory for many-electron systems strongly coupled to quantized electromagnetic modes of a microcavity is proposed. It is shown that the electron-photon wave function is a unique functional of the…

Mesoscale and Nanoscale Physics · Physics 2013-12-10 I. V. Tokatly

Effective field theory (EFT) methods are applied to density functional theory (DFT) as part of a program to systematically go beyond mean-field approaches to medium and heavy nuclei. A system of fermions with short-range, natural…

Nuclear Theory · Physics 2007-05-23 S. J. Puglia , A. Bhattacharyya , R. J. Furnstahl

The exchange-correlation potential experienced by an electron in the free space adjacent to a solid surface or to a low-dimensional system defines the fundamental image states and is generally important in surface- and nano-science. Here we…

Mesoscale and Nanoscale Physics · Physics 2016-06-01 V. U. Nazarov

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

The exact interaction energy of a many-electron system is determined by the electron pair density, which is not well-approximated in standard Kohn-Sham density functional models. Here we study the (complicated but well-defined) exact…

Chemical Physics · Physics 2015-08-07 Huajie Chen , Gero Friesecke

DFT calculations have become widespread in both chemistry and materials, because they usually provide useful accuracy at much lower computational cost than wavefunction-based methods. All practical DFT calculations require an approximation…

Chemical Physics · Physics 2022-03-15 Eunji Sim , Suhwan Song , Stefan Vuckovic , Kieron Burke

Perdew et al. [Phys. Rev. Lett 49, 1691 (1982)] discovered and proved two different properties of exact Kohn-Sham density functional theory (DFT): (i) The exact total energy versus particle number is a series of linear segments between…

Other Condensed Matter · Physics 2015-03-13 Tamar Stein , Jochen Autschbach , Niranjan Govind , Leeor Kronik , Roi Baer