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@ARTICLE{Han:58667,
author = {Han, B. and Li, Z. and Wandlowski, Th. and Blaszcyk, A. and
Mayor, M.},
title = {{P}otential-induced redox {S}witching in {V}iologen
{S}elf-assembled {M}onolayers - {A}n {ATR}-{SEIRAS}
{A}pproach},
journal = {The journal of physical chemistry / C},
volume = {111},
issn = {1932-7447},
address = {Washington, DC},
publisher = {Soc.},
reportid = {PreJuSER-58667},
pages = {13855 - 13863},
year = {2007},
note = {Record converted from VDB: 12.11.2012},
abstract = {Monolayers of viologens
(N-alkyl-N'-(n-thioalkyl)-4,4'-bipyridinium bromide, n = 6,
8, 10) have been self-assembled from ethanolic solution onto
gold substrates. Their structure and redox functionality
were studied by cyclic voltammetry and in situ ATR-SEIRAS.
Voltammetric experiments revealed that the first redox
process, V2+ <-> V center dot+, is reversible, whereas the
second redox process, V center dot+ <-> V-0, is quasi
reversible. The V2+ adlayer exhibits a sandwich-like
structure. Van der Waals interactions between the alkyl
chains lead to two well-ordered hydrophobic layers, with the
redox-active bipyridinium unit enclosed in between. The
alkyl chains are aligned in an all-trans configuration in a
tilted orientation with respect to the surface normal and
exhibit a slight conformational disorder. The long axis of
the central bipyridinium rings is also tilted. The alignment
of V2+ is stabilized by interplanar pi-pi stacking and
electrostatic coulomb interactions. Both monomers and dimers
of V center dot+ coexist in the V center dot+ adlayer. The
molecular alignment of the V center dot+ adlayer is
stabilized by the strong vibronic coupling within the dimers
and the pi-pi stacking between the monomers. Increasing
length of the alkyl chain results in more tilted
bipyridinium units, and favors both the dimerization and the
alignment of V center dot+ within the SAMs. The complex
reaction, V2+ - V center dot+, is described as electron
transport from the electrode to the V2+ moiety followed by
the dimerization of V center dot+, the delocalization of the
radical electrons, and the migration of coadsorbed ClO4-
anions.},
keywords = {J (WoSType)},
cin = {IBN-3 / CNI / JARA-FIT},
ddc = {540},
cid = {I:(DE-Juel1)VDB801 / I:(DE-Juel1)VDB381 /
$I:(DE-82)080009_20140620$},
pnm = {Grundlagen für zukünftige Informationstechnologien},
pid = {G:(DE-Juel1)FUEK412},
shelfmark = {Chemistry, Physical / Nanoscience $\&$ Nanotechnology /
Materials Science, Multidisciplinary},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000249501800032},
doi = {10.1021/jp073208g},
url = {https://juser.fz-juelich.de/record/58667},
}