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@ARTICLE{Muchova:616885,
author = {Muchova, Eva and Gopakumar, Geethanjali and Unger, Isaak
and Oehrwall, Gunnar and Ceolin, Denis and Trinter, Florian
and Wilkinson, Iain and Chatzigeorgiou, E. and Slavicek,
Petr and Hergenhahn, Uwe and Winter, Bernd and Caleman, Carl
and Bjoerneholm, Olle},
title = {{A}ttosecond formation of charge-transfer-to-solvent states
of aqueous ions probed using the core-hole-clock technique},
journal = {Nature Communications},
volume = {15},
number = {1},
issn = {2041-1723},
address = {[London]},
publisher = {Nature Publishing Group UK},
reportid = {PUBDB-2024-06566},
pages = {8903},
year = {2024},
note = {Open Access},
abstract = {Charge transfer between molecules lies at the heart of many
chemical processes. Here, we focus on the ultrafast electron
dynamics associated with the formation of
charge-transfer-to-solvent (CTTS) states following X-ray
absorption in aqueous solutions of Na+, Mg2+, and Al3+ ions.
To explore the formation of such states in the aqueous
phase, liquid-jet photoemission spectroscopy is employed.
Using the core-hole-clock method, based on Auger–Meitner
(AM) decay upon 1s excitation or ionization of the
respective ions, upper limits are estimated for the
metal-atom electron delocalization times to the neighboring
water molecules. These delocalization processes represent
the first steps in the formation of hydrated electrons,
which are determined to take place on a timescale ranging
from several hundred attoseconds (as) below the 1s
ionization threshold to only 20 as far above the 1s
ionization threshold. The decrease in the delocalization
times as a function of the photon energy is continuous. This
indicates that the excited electrons remain in the vicinity
of the studied ions even above the ionization threshold,
i.e., metal-ion electronic resonances associated with the
CTTS state manifolds are formed. The three studied
isoelectronic ions exhibit quantitative differences in their
electron energetics and delocalization times, which are
linked to the character of the respective excited states.},
cin = {DOOR ; HAS-User / FS-PETRA-S},
ddc = {500},
cid = {I:(DE-H253)HAS-User-20120731 /
I:(DE-H253)FS-PETRA-S-20210408},
pnm = {631 - Matter – Dynamics, Mechanisms and Control
(POF4-631) / 6G3 - PETRA III (DESY) (POF4-6G3) /
FS-Proposal: I-20190339 (I-20190339) / AQUACHIRAL - Chiral
aqueous-phase chemistry (883759) / DFG project
G:(GEPRIS)509471550 - Dynamik photoionisations-induzierter
Prozesse in laser-präparierten Molekülen in der Gasphase
und der wässrigen Phase (509471550)},
pid = {G:(DE-HGF)POF4-631 / G:(DE-HGF)POF4-6G3 /
G:(DE-H253)I-20190339 / G:(EU-Grant)883759 /
G:(GEPRIS)509471550},
experiment = {EXP:(DE-H253)P-P04-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:39406706},
UT = {WOS:001337260300003},
doi = {10.1038/s41467-024-52740-5},
url = {https://bib-pubdb1.desy.de/record/616885},
}