Attosecond spectroscopy reveals alignment dependent core-hole dynamics in the ICl molecule

Hugo J. B. Marroux (), Ashley P. Fidler, Aryya Ghosh, Yuki Kobayashi, Kirill Gokhberg, Alexander I. Kuleff, Stephen R. Leone () and Daniel M. Neumark ()
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Hugo J. B. Marroux: University of California
Ashley P. Fidler: University of California
Aryya Ghosh: Universität Heidelberg
Yuki Kobayashi: University of California
Kirill Gokhberg: Universität Heidelberg
Alexander I. Kuleff: Universität Heidelberg
Stephen R. Leone: University of California
Daniel M. Neumark: University of California

Nature Communications, 2020, vol. 11, issue 1, 1-8

Abstract: Abstract The removal of electrons located in the core shells of molecules creates transient states that live between a few femtoseconds to attoseconds. Owing to these short lifetimes, time-resolved studies of these states are challenging and complex molecular dynamics driven solely by electronic correlation are difficult to observe. Here, we obtain few-femtosecond core-excited state lifetimes of iodine monochloride by using attosecond transient absorption on iodine 4d−16p transitions around 55 eV. Core-level ligand field splitting allows direct access of excited states aligned along and perpendicular to the ICl molecular axis. Lifetimes of 3.5 ± 0.4 fs and 4.3 ± 0.4 fs are obtained for core-hole states parallel to the bond and 6.5 ± 0.6 fs and 6.9 ± 0.6 fs for perpendicular states, while nuclear motion is essentially frozen on this timescale. Theory shows that the dramatic decrease of lifetime for core-vacancies parallel to the covalent bond is a manifestation of non-local interactions with the neighboring Cl atom of ICl.

Date: 2020
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DOI: 10.1038/s41467-020-19496-0

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