• DOI:10.1038/s41467-020-19496-0
• Corpus ID: 211066343

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

@article{Marroux2020AttosecondSR,
  title={Attosecond spectroscopy reveals alignment dependent core-hole dynamics in the ICl molecule},
  author={Hugo J. B. Marroux and Ashley P. Fidler and Aryya Ghosh and Yuki Kobayashi and Kirill Gokhberg and Alexander I. Kuleff and Stephen R. Leone and Daniel M. Neumark},
  journal={Nature Communications},
  year={2020},
  volume={11}
}

• Hugo J. B. Marroux, A. Fidler, +5 authors D. Neumark
• Published 6 February 2020
• Physics, Chemistry
• Nature Communications

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. Here the authors report a study measuring lifetimes of core-hole states of ICl molecule using attosecond transient absorption spectroscopy. They find that lifetimes depend on the alignment of the orbital relative to the molecular axis.