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@ARTICLE{Haldrup:297390,
author = {Haldrup, Kristoffer and Gawelda, Wojciech and Abela, Rafael
and Alonso-Mori, Roberto and Bergmann, Uwe and Bordage,
Amélie and Cammarata, Marco and Canton, Sophie and Dohn,
Asmus Ougaard and van Driel, Tim Brandt and Fritz, David M.
and Galler, Andreas and Glatzel, Pieter and Harlang, Tobias
and Kjær, Kasper S. and Lemke, Henrik T. and Møller, Klaus
B. and Németh, Zoltán and Pápai, Mátyás and Sas,
Norbert and Uhlig, Jens and Zhu, Diling and Vankó, György
and Sundström, Villy and Nielsen, Martin M. and Bressler,
Christian},
title = {{O}bserving {S}olvation {D}ynamics with {S}imultaneous
{F}emtosecond {X}-ray {E}mission {S}pectroscopy and {X}-ray
{S}cattering},
journal = {The journal of physical chemistry / B},
volume = {120},
number = {6},
issn = {1520-5207},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {PUBDB-2016-01853},
pages = {1158 - 1168},
year = {2016},
abstract = {In liquid phase chemistry dynamic solute–solvent
interactions often govern the path, ultimate outcome, and
efficiency of chemical reactions. These steps involve
many-body movements on subpicosecond time scales and thus
ultrafast structural tools capable of capturing both
intramolecular electronic and structural changes, and local
solvent structural changes are desired. We have studied the
intra- and intermolecular dynamics of a model chromophore,
aqueous $[Fe(bpy)_{3}]^{2+}$, with complementary X-ray tools
in a single experiment exploiting intense XFEL radiation as
a probe. We monitored the ultrafast structural rearrangement
of the solute with X-ray emission spectroscopy, thus
establishing time zero for the ensuing X-ray diffuse
scattering analysis. The simultaneously recorded X-ray
diffuse scattering patterns reveal slower subpicosecond
dynamics triggered by the intramolecular structural dynamics
of the photoexcited solute. By simultaneous combination of
both methods only, we can extract new information about the
solvation dynamic processes unfolding during the first
picosecond (ps). The measured bulk solvent density increase
of 0.2\% indicates a dramatic change of the solvation shell
around each photoexcited solute, confirming previous ab
initio molecular dynamics simulations. Structural changes in
the aqueous solvent associated with density and temperature
changes occur with ∼1 ps time constants, characteristic
for structural dynamics in water. This slower time scale of
the solvent response allows us to directly observe the
structure of the excited solute molecules well before the
solvent contributions become dominant.},
cin = {Eur.XFEL / FS-SCS},
ddc = {530},
cid = {$I:(DE-H253)Eur_XFEL-20120731$ /
I:(DE-H253)FS-SCS-20131031},
pnm = {6215 - Soft Matter, Health and Life Sciences (POF3-621) /
6G13 - XFEL (POF3-622)},
pid = {G:(DE-HGF)POF3-6215 / G:(DE-HGF)POF3-6G13},
experiment = {EXP:(DE-H253)XFEL-FXE-20150101},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000370678500013},
pubmed = {pmid:26783685},
doi = {10.1021/acs.jpcb.5b12471},
url = {https://bib-pubdb1.desy.de/record/297390},
}