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@ARTICLE{Toher:14833,
author = {Toher, C. and Temirov, R. and Greuling, A. and Pump, F. and
Kaczmarski, M. and Cuniberti, G. and Rohlfing, M. and Tautz,
F.S.},
title = {{E}lectrical transport through a mechanically gated
molecular wire},
journal = {Physical review / B},
volume = {83},
number = {15},
issn = {1098-0121},
address = {College Park, Md.},
publisher = {APS},
reportid = {PreJuSER-14833},
pages = {155402},
year = {2011},
note = {Computational facilities were provided by the Zentrum fur
Informationsdienste und Hochleistungsrechnen (ZIH) at TU
Dresden and by the Julich Supercomputing Centre at the
Forschungszentrum Julich. We gratefully acknowledge the
financial support of the Deutsche Forschungsgemeinschaft in
the framework of the priority program SPP 1243, the South
Korean Ministry of Education, Science, and Technology
Program, Project No. WCU ITCE No. R31-2008-000-10100-0, and
from ECEMP, the European Center for Emerging Materials and
Processes Dresden (Project No. A2).},
abstract = {A surface-adsorbed molecule is contacted with the tip of a
scanning tunneling microscope (STM) at a predefined atom. On
tip retraction, the molecule is peeled off the surface.
During this experiment, a two-dimensional differential
conductance map is measured on the plane spanned by the bias
voltage and the tip-surface distance. The conductance map
demonstrates that tip retraction leads to mechanical gating
of the molecular wire in the STM junction. The experiments
are compared with a detailed ab initio simulation. We find
that density functional theory (DFT) in the local density
approximation (LDA) describes the tip-molecule contact
formation and the geometry of the molecular junction
throughout the peeling process with predictive power.
However, a DFT-LDA-based transport simulation following the
nonequilibrium Green's function (NEGF) formalism fails to
describe the behavior of the differential conductance as
found in experiment. Further analysis reveals that this
failure is due to the mean-field description of electron
correlation in the local density approximation. The results
presented here are expected to be of general validity and
show that, for a wide range of common wire configurations,
simulations which go beyond the mean-field level are
required to accurately describe current conduction through
molecules. Finally, the results of the present study
illustrate that well-controlled experiments and concurrent
ab initio transport simulations that systematically sample a
large configuration space of molecule-electrode couplings
allow the unambiguous identification of correlation
signatures in experiment.},
keywords = {J (WoSType)},
cin = {PGI-3 / JARA-FIT},
ddc = {530},
cid = {I:(DE-Juel1)PGI-3-20110106 / $I:(DE-82)080009_20140620$},
pnm = {Grundlagen für zukünftige Informationstechnologien},
pid = {G:(DE-Juel1)FUEK412},
shelfmark = {Physics, Condensed Matter},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000289053300004},
doi = {10.1103/PhysRevB.83.155402},
url = {https://juser.fz-juelich.de/record/14833},
}