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@ARTICLE{Hallmann:89182,
author = {Hallmann, J. and Morgenroth, W. and Paulmann, C. and
Davaasambuu, J. and Kong, Q. and Wulff, M. and Techert, S.
and DESY},
title = {{T}ime-resolved x-ray diffraction of the photochromic
alpha-styrylpyrylium {T}rifluoromethanesulfonate crystal
films reveals ultrafast structural switching},
journal = {Journal of the American Chemical Society},
volume = {131},
issn = {0002-7863},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {PHPPUBDB-17382},
pages = {15018-15025},
year = {2009},
note = {© American Chemical Society},
abstract = {The ultrafast structural dynamics of the [2+2]
photocycloaddition of alpha-styrylpyrylium
trifluoromethanesulfonate (TFMS) has been studied in great
detail. During the photoreaction, optical and infrared
spectroscopy confirms that crystals of alpha-styrylpyrylium
change color. Since the reaction is reversible, it has been
suggested to be used as an organic holographic storage
device. The present photocrystallographic studies (with high
spatial resolution) allow for an electron density analysis
of the overall reaction kinetics, revealing the mechanism of
bond-breaking and bond-formation. It could furthermore be
proved how the reaction is influenced by the rearrangement
of the surrounding moieties. Picosecond time-resolved X-ray
diffraction studies allow for the monitoring the
photoreaction in crystalline thin films under experimental
conditions where the transformation times are greatly
enhanced. These investigations are discussed in the context
of the photocrystallographic results. It has been found that
alpha-styrylpyrylium TFMS undergoes an ultrafast
photoreaction to the dimer product state and back-reaction
to the monomer reactant state which is temperature driven.
The present experiments indicate that TFMS reacts on time
scales which are the fundamental limiting ones of
two-quantum systems and therefore has the potential to be
used as an ultrafast organic molecular switcher.},
keywords = {Alkanesulfonates: chemistry / Crystallography, X-Ray /
Dimerization / Electrons / Photochemical Processes / Pyrans:
chemistry / Spectrophotometry, Infrared / Styrenes:
chemistry / Temperature / Time Factors / Alkanesulfonates
(NLM Chemicals) / Pyrans (NLM Chemicals) / Styrenes (NLM
Chemicals) / alpha-styrylpyrylium (NLM Chemicals)},
cin = {HASYLAB(-2012) / FS-SCS},
ddc = {540},
cid = {$I:(DE-H253)HASYLAB_-2012_-20130307$ /
I:(DE-H253)FS-SCS-20131031},
pnm = {DORIS Beamline D3 (POF1-550) / DORIS Beamline F1
(POF1-550)},
pid = {G:(DE-H253)POF1-D3-20130405 / G:(DE-H253)POF1-F1-20130405},
experiment = {EXP:(DE-H253)D-D3-20150101 / EXP:(DE-H253)D-F1-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:19824735},
UT = {WOS:000271271800077},
doi = {10.1021/ja905484u},
url = {https://bib-pubdb1.desy.de/record/89182},
}