TY  - JOUR
AU  - Muchova, Eva
AU  - Gopakumar, Geethanjali
AU  - Unger, Isaak
AU  - Oehrwall, Gunnar
AU  - Ceolin, Denis
AU  - Trinter, Florian
AU  - Wilkinson, Iain
AU  - Chatzigeorgiou, E.
AU  - Slavicek, Petr
AU  - Hergenhahn, Uwe
AU  - Winter, Bernd
AU  - Caleman, Carl
AU  - Bjoerneholm, Olle
TI  - Attosecond formation of charge-transfer-to-solvent states of aqueous ions probed using the core-hole-clock technique
JO  - Nature Communications
VL  - 15
IS  - 1
SN  - 2041-1723
CY  - [London]
PB  - Nature Publishing Group UK
M1  - PUBDB-2024-06566
SP  - 8903
PY  - 2024
N1  - Open Access
AB  - 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.
LB  - PUB:(DE-HGF)16
C6  - pmid:39406706
UR  - <Go to ISI:>//WOS:001337260300003
DO  - DOI:10.1038/s41467-024-52740-5
UR  - https://bib-pubdb1.desy.de/record/616885
ER  -