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A fundamental property of a quantum system driven by an external field is that when the field is turned off the positions of its response frequencies are independent of the time at which the field is turned off. We show that this leads to…

Chemical Physics · Physics 2015-05-29 Johanna I. Fuks , Kai Luo , Ernesto D. Sandoval , Neepa T. Maitra

Specific matrix elements of exchange and correlation kernels in time-dependent density-functional theory are computed. The knowledge of these matrix elements not only constraints approximate time-dependent functionals, but also allows to…

Materials Science · Physics 2009-10-31 X. Gonze , M. Scheffler

The frequency-dependent exchange-correlation potential, which appears in the usual Kohn-Sham formulation of a time-dependent linear response problem, is a strongly nonlocal functional of the density, so that a consistent local density…

Condensed Matter · Physics 2009-10-28 G. Vignale , Walter Kohn

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

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

We employ the density matrix renormalization group to construct the exact time-dependent exchange correlation potential for an impurity model with an applied transport voltage. Even for short-ranged interaction we find an infinitely…

Mesoscale and Nanoscale Physics · Physics 2017-09-13 Peter Schmitteckert , Michael Dzierzawa , Peter Schwab

We identify the key property that the exchange-correlation (XC) kernel of time-dependent density functional theory must have in order to describe long-range charge-transfer excitations. We show that the discontinuity of the XC potential as…

Mesoscale and Nanoscale Physics · Physics 2015-05-30 M. Hellgren , E. K. U. Gross

A review of the approximations in any time-dependent density functional calculation of excitation energies is given. The single-pole approximation for the susceptibility is used to understand errors in popular approximations for the…

Materials Science · Physics 2007-05-23 Kieron Burke , Martin Petersilka , E. K. U. Gross

Most present applications of time-dependent density functional theory use adiabatic functionals, i.e. the effective potential at time t is determined solely by the density at the same time. This paper discusses a method that aims to go…

Strongly Correlated Electrons · Physics 2009-11-10 Yair Kurzweil , Roi Baer

The performance of several common approximations for the exchange-correlation kernel within time-dependent density-functional theory is tested for elementary excitations in the homogeneous electron gas. Although the adiabatic local-density…

Materials Science · Physics 2007-05-23 Krzysztof Tatarczyk , Arno Schindlmayr , Matthias Scheffler

We propose a systematic and constructive way to determine the exchange-correlation potentials of density-functional theories including vector potentials. The approach does not rely on energy or action functionals. Instead it is based on…

In time-dependent density-functional theory, exchange and correlation (xc) beyond the adiabatic local density approximation can be described in terms of viscoelastic stresses in the electron liquid. In the time domain, this leads to a…

Mesoscale and Nanoscale Physics · Physics 2009-11-10 H. O. Wijewardane , C. A. Ullrich

We present a detailed study of the exact-exchange (EXX) kernel of time-dependent density functional theory with an emphasis on its discontinuity at integer particle numbers. It was recently found that this exact property leads to sharp…

Chemical Physics · Physics 2015-06-17 M. Hellgren , E. K. U. Gross

A semi-relativistic density-functional theory that includes spin-orbit couplings and Zeeman fields on equal footing with the electromagnetic potentials, is an appealing framework to develop a unified first-principles computational approach…

Materials Science · Physics 2017-09-13 S. Pittalis , G. Vignale , F. G. Eich

We study a simple but useful test for neural exchange-correlation (XC) functionals: can a neural model reproduce an established XC functional when it is used self-consistently? We call this test functional cloning. The model is trained at…

The exact exchange-correlation (xc) kernel $f_\mathrm{xc}(x,x',\omega)$ of linear response time-dependent density functional theory is computed over a wide range of frequencies, for three canonical one-dimensional finite systems. Methods…

Materials Science · Physics 2021-04-07 N. D. Woods , M. T. Entwistle , R. W. Godby

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

For two prototype systems, we calculate the exact exchange-correlation kernels $f_{\mathrm{xc}}(x,x',\omega)$ of time-dependent density functional theory. $f_{\mathrm{xc}}$, the key quantity for optical absorption spectra of electronic…

Other Condensed Matter · Physics 2019-04-10 Mike Entwistle , Rex Godby

The dynamical, long-wavelength longitudinal and transverse exchange-correlation potentials for a homogeneous electron gas are evaluated in a microscopic model based on an approximate decoupling of the equation of motion for the…

Condensed Matter · Physics 2009-10-30 S. Conti , R. Nifosi' , M P Tosi

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…

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