Journal Article

PUBDB-2024-06566

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Attosecond formation of charge-transfer-to-solvent states of aqueous ions probed using the core-hole-clock technique

Muchova, E. (Corresponding author)Extern*XFEL.EU* ; Gopakumar, G.Extern*XFEL.EU* ; Unger, I.Extern*XFEL.EU*DESY* ; Oehrwall, G.Extern* ; Ceolin, D.Extern* ; Trinter, F.Extern*XFEL.EU* ; Wilkinson, I.Extern* ; Chatzigeorgiou, E. ; Slavicek, P.Extern*XFEL.EU* ; Hergenhahn, U.Extern* ; Winter, B.Extern* ; Caleman, C.CFEL*DESY* ; Bjoerneholm, O. (Corresponding author)Extern*XFEL.EU*

2024
Nature Publishing Group UK [London]

This record in other databases:        

Please use a persistent id in citations: doi:10.1038/s41467-024-52740-5  doi:10.3204/PUBDB-2024-06566

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.

Note: Open Access

---

Contributing Institute(s):

1. DOOR-User (DOOR ; HAS-User)
2. PETRA-S (FS-PETRA-S)

Research Program(s):

1. 631 - Matter – Dynamics, Mechanisms and Control (POF4-631) (POF4-631)
2. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
3. FS-Proposal: I-20190339 (I-20190339) (I-20190339)
4. AQUACHIRAL - Chiral aqueous-phase chemistry (883759) (883759)
5. DFG project G:(GEPRIS)509471550 - Dynamik photoionisations-induzierter Prozesse in laser-präparierten Molekülen in der Gasphase und der wässrigen Phase (509471550) (509471550)

Experiment(s):

1. PETRA Beamline P04 (PETRA III)

Appears in the scientific report 2024

---

Database coverage:
; ; ; ; Article Processing Charges ; BIOSIS Previews ; Biological Abstracts ; Clarivate Analytics Master Journal List ; Current Contents - Agriculture, Biology and Environmental Sciences ; Current Contents - Life Sciences ; Current Contents - Physical, Chemical and Earth Sciences ; DOAJ Seal ; Essential Science Indicators ; Fees ; IF >= 15 ; JCR ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection ; Zoological Record

---