Tracing charge transfer in argon dimers by XUV-pump IR-probe experiments at FLASH

Charge transfer (CT) at avoided crossings of excited ionized states of argon dimers is observed using a two-color pump-probe experiment at the free-electron laser in Hamburg (FLASH). The process is initiated by the absorption of three 27-eV-photons from the pump pulse, which leads to the population...

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Bibliographic Details
Published in:The Journal of chemical physics 2019-08, Vol.151 (8), p.084314-084314
Main Authors: Schmid, Georg, Schnorr, Kirsten, Augustin, Sven, Meister, Severin, Lindenblatt, Hannes, Trost, Florian, Liu, Yifan, Miteva, Tsveta, Gisselbrecht, Mathieu, Düsterer, Stefan, Redlin, Harald, Treusch, Rolf, Gokhberg, Kirill, Kuleff, Alexander I., Cederbaum, Lorenz S., Schröter, Claus Dieter, Pfeifer, Thomas, Moshammer, Robert
Format: Article
Language:English
Subjects:
Argon
Argon ions
Atom and Molecular Physics and Optics
Atom- och molekylfysik och optik
Charge transfer
Chemical Sciences
Dimers
Free electron lasers
Fysik
Fysikalisk kemi
Infrared lasers
Kemi
Natural Sciences
Naturvetenskap
Physical Chemistry
Physical Sciences
Teoretisk kemi
Theoretical Chemistry
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Summary:Charge transfer (CT) at avoided crossings of excited ionized states of argon dimers is observed using a two-color pump-probe experiment at the free-electron laser in Hamburg (FLASH). The process is initiated by the absorption of three 27-eV-photons from the pump pulse, which leads to the population of Ar2+*–Ar states. Due to nonadiabatic coupling between these one-site doubly ionized states and two-site doubly ionized states of the type Ar+*–Ar+, CT can take place leading to the population of the latter states. The onset of this process is probed by a delayed infrared (800 nm) laser pulse. The latter ionizes the dimers populating repulsive Ar2+ –Ar+ states, which then undergo a Coulomb explosion. From the delay-dependent yields of the obtained Ar2+ and Ar+ ions, the lifetime of the charge-transfer process is extracted. The obtained experimental value of (531 ± 136) fs agrees well with the theoretical value computed from Landau-Zener probabilities.
ISSN:0021-9606
1089-7690
DOI:10.1063/1.5116234