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@ARTICLE{VelazquezGarcia:618863,
author = {Velazquez Garcia, Jose and Basuroy, Krishnayan and Wong,
Joanne and Demeshko, Serhiy and Meyer, Franc and Kim, Insik
and Henning, Robert and Staechelin, Yannic and Lange, Holger
and Techert, Simone},
title = {{O}ut-of-equilibrium dynamics of a grid-like {F}e({II})spin
crossover dimer triggered by a two-photonexcitation},
journal = {Chemical science},
volume = {15},
number = {33},
issn = {2041-6520},
address = {Cambridge},
publisher = {RSC},
reportid = {PUBDB-2024-07201},
pages = {13531-13540},
year = {2024},
abstract = {The application of two-photon excitation (TPE) in the study
of light-responsive materials holds immense potential due to
its deeper penetration and reduced photodamage. Despite
these benefits, TPE has been underutilised in the
investigation of the photoinduced spin crossover (SCO)
phenomenon. Here, we employ TPE to delve into the
out-of-equilibrium dynamics of a SCO FeII dimer of the form
[FeII(HL)$_2$]$_2$(BF$_4$)$_4$·2MeCN (HL =
3,5-bis{6-(2,2′-bipyridyl)}pyrazole). Optical transient
absorption (OTA) spectroscopy in solution proves that the
same dynamics take place under both one-photon excitation
(OPE) and TPE. The results show the emergence of the
photoinduced high spin state in less than 2 ps and with a
lifetime of 147 ns. Time-resolved photocrystallography
(TRXRD) reveals a single molecular reorganisation within the
first 500 ps following TPE. Additionally, variable
temperature single crystal X-ray diffraction (VTSCXRD) and
magnetic susceptibility measurements confirm that the
thermal transition is silenced by the solvent. While the
results of the OTA and TRXRD utilising TPE are intriguing,
the high pump fluencies required to excite enough metal
centres to the high spin state may impair its practical
application. Nonetheless, this study sheds light on the
potential of TPE for the investigation of the
out-of-equilibrium dynamics of SCO complexes.},
cin = {FS-SCS},
ddc = {540},
cid = {I:(DE-H253)FS-SCS-20131031},
pnm = {631 - Matter – Dynamics, Mechanisms and Control
(POF4-631) / 6G3 - PETRA III (DESY) (POF4-6G3) / SFB 1073
B06 - Echtzeituntersuchungen der optischen Anregung in
oligonuklearen Metallkomplexen mit schaltbaren Spin- und
Ladungszuständen (B06) (240171831) / SFB 1073 C02 - In-situ
hochauflösende Untersuchung des aktiven Zustands bei der
(photo-) elektrochemischen Wasserspaltung (C02) (240172646)},
pid = {G:(DE-HGF)POF4-631 / G:(DE-HGF)POF4-6G3 /
G:(GEPRIS)240171831 / G:(GEPRIS)240172646},
experiment = {EXP:(DE-H253)P-P11-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:39183926},
UT = {WOS:001280613400001},
doi = {10.1039/d4sc02933j},
url = {https://bib-pubdb1.desy.de/record/618863},
}