Attosecond spectroscopy reveals alignment dependent core-hole dynamics in the ICl molecule
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...
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| Hauptverfasser: | , , , , , , , |
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| Dokumenttyp: | Article (Journal) |
| Sprache: | Englisch |
| Veröffentlicht: |
16 November 2020
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| In: |
Nature Communications
Year: 2020, Jahrgang: 11 |
| ISSN: | 2041-1723 |
| DOI: | 10.1038/s41467-020-19496-0 |
| Online-Zugang: | Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1038/s41467-020-19496-0 Verlag, lizenzpflichtig, Volltext: https://www.nature.com/articles/s41467-020-19496-0 
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| Verfasserangaben: | Hugo J.B. Marroux, Ashley P. Fidler, Aryya Ghosh, Yuki Kobayashi, Kirill Gokhberg, Alexander I. Kuleff, Stephen R. Leone & Daniel M. Neumark |
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| 520 | |a 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. | ||
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