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.
Skip Nav Destination
Article navigation
14 May 2014
Research Article|
March 19 2014
Ultra-nonlocality in density functional theory for photo-emission spectroscopy
A.-M. Uimonen;
A.-M. Uimonen
1Department of Physics, Nanoscience Center,
University of Jyväskylä
, Survontie 9, 40014 Jyväskylä, Finland
Search for other works by this author on:
G. Stefanucci;
G. Stefanucci
2Dipartimento di Fisica,
Universitá di Roma Tor Vergata
, Via della Ricerca Scientifica, 00133 Rome, Italy
3
INFN
, Laboratori Nazionali di Frascati, Via E. Fermi 40, 00044 Frascati, Italy
4
European Theoretical Spectroscopy Facility (ETSF)
, Louvain-la Neuve, Belgium
Search for other works by this author on:
R. van Leeuwen
R. van Leeuwen
1Department of Physics, Nanoscience Center,
University of Jyväskylä
, Survontie 9, 40014 Jyväskylä, Finland
4
European Theoretical Spectroscopy Facility (ETSF)
, Louvain-la Neuve, Belgium
Search for other works by this author on:
J. Chem. Phys. 140, 18A526 (2014)
Article history
Received:
November 26 2013
Accepted:
February 27 2014
Citation
A.-M. Uimonen, G. Stefanucci, R. van Leeuwen; Ultra-nonlocality in density functional theory for photo-emission spectroscopy. J. Chem. Phys. 14 May 2014; 140 (18): 18A526. https://doi.org/10.1063/1.4868114
Download citation file:
Pay-Per-View Access
$40.00
Sign In
You could not be signed in. Please check your credentials and make sure you have an active account and try again.
Citing articles via
DeePMD-kit v2: A software package for deep potential models
Jinzhe Zeng, Duo Zhang, et al.
CREST—A program for the exploration of low-energy molecular chemical space
Philipp Pracht, Stefan Grimme, et al.
Dielectric profile at the Pt(111)/water interface
Jia-Xin Zhu, Jun Cheng, et al.
Related Content
Design of effective kernels for spectroscopy and molecular transport: Time-dependent current–density-functional theory
J. Chem. Phys. (February 2011)
Towards time-dependent current-density-functional theory in the non-linear regime
J. Chem. Phys. (February 2015)
On the role of the nonlocal Hartree–Fock exchange in ab initio quantum transport: H 2 in Pt nanocontacts revisited
J. Chem. Phys. (July 2008)
Communications: On the relation between the scalar and tensor exchange-correlation kernels of the time-dependent density-functional theory
J. Chem. Phys. (July 2010)
Current density partitioning in time-dependent current density functional theory
J. Chem. Phys. (March 2014)