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

Author

Listed:
  • Hugo J. B. Marroux

    (University of California
    Lawrence Berkeley National Laboratory
    ISIC, FSB)

  • Ashley P. Fidler

    (University of California
    Lawrence Berkeley National Laboratory)

  • Aryya Ghosh

    (Universität Heidelberg)

  • Yuki Kobayashi

    (University of California)

  • Kirill Gokhberg

    (Universität Heidelberg)

  • Alexander I. Kuleff

    (Universität Heidelberg
    ELI-ALPS)

  • Stephen R. Leone

    (University of California
    Lawrence Berkeley National Laboratory
    University of California)

  • Daniel M. Neumark

    (University of California
    Lawrence Berkeley National Laboratory)

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.

Suggested Citation

  • Hugo J. B. Marroux & Ashley P. Fidler & Aryya Ghosh & Yuki Kobayashi & Kirill Gokhberg & Alexander I. Kuleff & Stephen R. Leone & Daniel M. Neumark, 2020. "Attosecond spectroscopy reveals alignment dependent core-hole dynamics in the ICl molecule," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-19496-0
    DOI: 10.1038/s41467-020-19496-0
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