Ultra-nonlocality in density functional theory for photo-emission spectroscopy

Abstract

We derive an exact expression for the photo-current of photo-emission spectroscopy using time-dependent current density functional theory (TDCDFT). This expression is given as an integral over the Kohn-Sham spectral function renormalized by effective potentials that depend on the exchange-correlation kernel of current density functional theory. We analyze in detail the physical content of this expression by making a connection between the density-functional expression and the diagrammatic expansion of the photo-current within many-body perturbation theory. We further demonstrate that the density functional expression does not provide us with information on the kinetic energy distribution of the photo-electrons. Such information can, in principle, be obtained from TDCDFT by exactly modeling the experiment in which the photo-current is split into energy contributions by means of an external electromagnetic field outside the sample, as is done in standard detectors. We find, however, that this procedure produces very nonlocal correlations between the exchange-correlation fields in the sample and the detector.

11 pages, 11 figures

References in corpus (7)

• A brief compendium of time-dependent density-functional theory
• Conserving Approximations in Time-Dependent Density Functional Theory
• Linear density response function within the time-dependent exact-exchange approximation
• Global fixed point proof of time-dependent density-functional theory
• Violation of the `Zero-Force Theorem' in the time-dependent Krieger-Li-Iafrate approximation
• Dynamical correction to linear Kohn-Sham conductances from static density functional theory
• A discontinuous functional for linear response time-dependent density functional theory: the exact-exchange kernel and approximate forms

Cited by in corpus (6)

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• Time-dependent many-body treatment of electron-boson dynamics: application to plasmon-accompanied photoemission
• One-step theory of pump-probe photoemission
• Mott metal-insulator transition from steady-state density functional theory
• One-step theory of two-photon photoemission