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

We derive an exact expression for the photocurrent 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...

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Bibliographic Details
Published in:The Journal of chemical physics 2014-05, Vol.140 (18), p.18A526-18A526
Main Authors: Uimonen, A-M, Stefanucci, G, van Leeuwen, R
Format: Article
Language:English
Subjects:
CURRENT DENSITY
DENSITY FUNCTIONAL METHOD
Density functional theory
ELECTROMAGNETIC FIELDS
EMISSION SPECTROSCOPY
Exchanging
INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
KINETIC ENERGY
Kinetic energy distribution
PERTURBATION THEORY
Photoelectric effect
Photoelectric emission
Physics
SIMULATION
SPECTRAL FUNCTIONS
Spectrum analysis
Time dependence
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Summary:We derive an exact expression for the photocurrent 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 photocurrent 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 photocurrent 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.
ISSN:0021-9606
1089-7690
DOI:10.1063/1.4868114