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@ARTICLE{Haags:1041428,
author = {Haags, Anja and Brandstetter, Dominik and Yang, Xiaosheng
and Egger, Larissa and Kirschner, Hans and Gottwald,
Alexander and Richter, Mathias and Koller, Georg and
Bocquet, François C. and Wagner, Christian and Ramsey,
Michael G. and Soubatch, Serguei and Puschnig, Peter and
Tautz, F. Stefan},
title = {{T}omographic identification of all molecular orbitals in a
wide binding-energy range},
journal = {Physical review / B},
volume = {111},
number = {16},
issn = {2469-9950},
address = {Woodbury, NY},
publisher = {Inst.},
reportid = {FZJ-2025-02241},
pages = {165402},
year = {2025},
abstract = {In the past decade, photoemission orbital tomography (POT)
has evolved into a powerful tool to investigate the
electronic structure of organic molecules adsorbed on
surfaces. Here we show that POT allows for the comprehensive
experimental identification of all molecular orbitals in a
substantial binding energy range of more than 10 eV. Making
use of the angular distribution of photoelectrons as a
function of binding-energy, we exemplify this by extracting
an orbital-resolved projected density of states for 15 𝜋
and 23 𝜎 orbitals from the experimental data of the
prototypical organic molecule bisanthene (C28H14) on a
Cu(110) surface. These experimental results for an
essentially complete set of orbitals within the given
binding-energy range serve as stringent benchmarks for
electronic structure methods, which we illustrate by
performing density functional calculations employing four
frequently used exchange-correlation functionals. By
computing the respective molecular-orbital-projected
densities of states, a one-to-one comparison with
experimental data for an unprecedented number of 38 orbital
energies became possible. The quantitative analysis of our
data reveals that the range-separated hybrid functional HSE
performs best for the investigated organic/metal interface.
At a more fundamental level, the remarkable agreement
between the experimental and the Kohn-Sham orbital energies
over a binding-energy range larger than 10 eV suggests
that—perhaps unexpectedly—Kohn-Sham orbitals approximate
Dyson orbitals, which would rigorously account for the
electron extraction process in photoemission spectroscopy
but are notoriously difficult to compute, in a much better
way than previously thought.},
cin = {PGI-3},
ddc = {530},
cid = {I:(DE-Juel1)PGI-3-20110106},
pnm = {5213 - Quantum Nanoscience (POF4-521) / Orbital Cinema -
Photoemission Orbital Cinematography: An ultrafast wave
function lab (101071259) / SFB 1083 A12 - Struktur und
Anregungen von hetero-epitaktischen Schichtsystemen aus
schwach wechselwirkenden 2D-Materialien und molekularen
Schichten (A12) (385975694) / CM3 - Controlled Mechanical
Manipulation of Molecules (757634)},
pid = {G:(DE-HGF)POF4-5213 / G:(EU-Grant)101071259 /
G:(GEPRIS)385975694 / G:(EU-Grant)757634},
typ = {PUB:(DE-HGF)16},
UT = {WOS:001460182600007},
doi = {10.1103/PhysRevB.111.165402},
url = {https://juser.fz-juelich.de/record/1041428},
}