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

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  • 2020-11-16
Published in:
  • Nature Communications. - Springer Science and Business Media LLC. - 2020, vol. 11, no. 1
General Biochemistry, Genetics and Molecular Biology
General Physics and Astronomy
General Chemistry
English AbstractThe 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.
Language
  • English
Open access status
gold
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Persistent URL
https://sonar.rero.ch/global/documents/225178
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