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An approximate solution to the time-dependent density functional theory (TDDFT) response equations for finite systems is developed, yielding corrections to the single-pole approximation. These explain why allowed Kohn-Sham transition…

Materials Science · Physics 2009-11-07 H. Appel , E. K. U. Gross , K. Burke

A new parameter-free approximation for the exchange-correlation kernel $f_{\rm xc}$ of time-dependent density functional theory is proposed. This kernel is expressed as an algorithm in which the exact Dyson equation for the response as well…

Materials Science · Physics 2015-05-28 S. Sharma , J. K. Dewhurst , A. Sanna , E. K. U. Gross

Fractional occupation numbers can be used in density functional theory to create a symmetric Kohn-Sham potential, resulting in orbitals with degenerate eigenvalues. We develop the corresponding perturbation theory and apply it to a system…

Materials Science · Physics 2016-09-09 Mark C. Palenik , Brett I. Dunlap

We obtain the conductance of a system of electrons connected to leads, within time-dependent density-functional theory, using a direct relation between the conductance and the density response function. Corrections to the non-interacting…

Materials Science · Physics 2007-10-04 P. Bokes , J. Jung , R. W. Godby

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

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

We establish the theoretical foundations for embedding a correlated wave function in an environment formed by Kohn-Sham orbitals. We show that introducing an approximation which equates two, in principle distinct, kinetic-energy functionals…

Chemical Physics · Physics 2026-03-06 Enzo Monino , Daria Drwal , Michał Hapka , Libor Veis , Katarzyna Pernal

The dynamical exchange-correlation kernel $f_{xc}$ of a non-uniform electron gas is an essential input for the time-dependent density functional theory of electronic systems. The long-wavelength behavior of this kernel is known to be of the…

Materials Science · Physics 2009-11-13 V. U. Nazarov , G. Vignale , Y. -C. Chang

We use voxel deep neural networks to predict energy densities and functional derivatives of electron kinetic energies for the Thomas-Fermi model and Kohn-Sham density functional theory calculations. We show that the ground-state electron…

Mesoscale and Nanoscale Physics · Physics 2022-01-24 Kevin Ryczko , Sebastian J. Wetzel , Roger G. Melko , Isaac Tamblyn

The 2p-3d core hole interaction in the L2,3 absorption spectra of the 3d transition metals is treated within time-dependent density functional theory (TDDFT). A simple three-level model explains the origin of the strong deviations from the…

Materials Science · Physics 2009-11-11 A. Scherz , E. K. U. Gross , H. Appel , C. Sorg , K. Baberschke , H. Wende , K. Burke

It is shown here that Kohn-Sham equations cannot be derived from Hohenberg-Kohn theory without an additional postulate. Assuming that a functional derivative with respect to total electron density exists leads in general to a theory…

Condensed Matter · Physics 2007-05-23 R. K. Nesbet

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…

We show that the analytic structure of the dynamical xc kernels of semiconductors and insulators can be sensed in terms of its poles which mark physically relevant frequencies of the system where the counter-phase motion of discrete…

Materials Science · Physics 2023-04-19 D. R. Gulevich , Ya. V. Zhumagulov , V. Kozin , I. V. Tokatly

A functional $E_{xc}[\rho(\r,\epsilon)]$ is presented, in which the exchange and correlation energy of an electron gas depends on the local density of occupied states. A simple local parametrization scheme is proposed, entirely from first…

Materials Science · Physics 2009-11-10 Jose M. Soler

A complete understanding of a material requires both knowledge of the excited states as well as of the ground state. In particular, the low energy excitations are of utmost importance while studying the electronic, magnetic, dynamical, and…

Materials Science · Physics 2019-01-30 N. Singh , P. Elliott , T. Nautiyal , J. K. Dewhurst , S. Sharma

In this work we have calculated excitation energies and photoionization cross sections of Be and Ne in the exact-exchange (EXX) approximation of time-dependent density functional theory (TDDFT). The main focus has been on the frequency…

Mesoscale and Nanoscale Physics · Physics 2015-05-14 Maria Hellgren , Ulf von Barth

Most approximate exchange-correlation functionals used within density functional theory are constructed as the sum of two distinct contributions for exchange and correlation. Separating the exchange component from the entire functional is…

Condensed Matter · Physics 2009-10-28 Claudia Filippi , C. J. Umrigar , Xavier Gonze

Density functional theory (DFT) is one of the most widely used tools to solve the many-body Schrodinger equation. The core uncertainty inside DFT theory is the exchange-correlation (XC) functional, the exact form of which is still unknown.…

Computational Physics · Physics 2019-10-15 Alexander Ryabov , Iskander Akhatov , Petr Zhilyaev

Machine learning is a powerful tool to design accurate, highly non-local, exchange-correlation functionals for density functional theory. So far, most of those machine learned functionals are trained for systems with an integer number of…

We propose exchanging the energy functionals in ground-state DFT with physically equivalent exact force expressions as a new promising route towards approximations to the exchange-correlation potential and energy. In analogy to the usual…

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