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@ARTICLE{Park:818202,
author = {Park, Kyoung-Duck and Muller, Eric A. and Kravtsov, Vasily
and Sass, Paul M. and Dreyer, Jens and Atkin, Joanna M. and
Raschke, Markus B.},
title = {{V}ariable-{T}emperature {T}ip-{E}nhanced {R}aman
{S}pectroscopy of {S}ingle-{M}olecule {F}luctuations and
{D}ynamics},
journal = {Nano letters},
volume = {16},
number = {1},
issn = {1530-6992},
address = {Washington, DC},
publisher = {ACS Publ.},
reportid = {FZJ-2016-04695},
pages = {479 - 487},
year = {2016},
abstract = {Structure, dynamics, and coupling involving
single-molecules determine function in catalytic, electronic
or biological systems. While vibrational spectroscopy
provides insight into molecular structure, rapid
fluctuations blur the molecular trajectory even in
single-molecule spectroscopy, analogous to spatial averaging
in measuring large ensembles. To gain insight into
intramolecular coupling, substrate coupling, and dynamic
processes, we use tip-enhanced Raman spectroscopy (TERS) at
variable and cryogenic temperatures, to slow and control the
motion of a single molecule. We resolve intrinsic line
widths of individual normal modes, allowing detailed and
quantitative investigation of the vibrational modes. From
temperature dependent line narrowing and splitting, we
quantify ultrafast vibrational dephasing, intramolecular
coupling, and conformational heterogeneity. Through
statistical correlation analysis of fluctuations of
individual modes, we observe rotational motion and spectral
fluctuations of the molecule. This work demonstrates
single-molecule vibrational spectroscopy beyond chemical
identification, opening the possibility for a complete
picture of molecular motion ranging from femtoseconds to
minutes.},
cin = {GRS Jülich ; German Research School for Simulation
Sciences},
ddc = {540},
cid = {I:(DE-Juel1)GRS-20100316},
pnm = {899 - ohne Topic (POF3-899)},
pid = {G:(DE-HGF)POF3-899},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000368322700074},
pubmed = {pmid:26679007},
doi = {10.1021/acs.nanolett.5b04135},
url = {https://juser.fz-juelich.de/record/818202},
}