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

Journal Article · · Nature Communications
 [1];  [1];  [2];  [3];  [2];  [4];  [5];  [1]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Div.
  2. Heidelberg Univ. (Germany). Theoretische Chemie
  3. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  4. Heidelberg Univ. (Germany). Theoretische Chemie; ELI-ALPS, Szeged (Hungary)
  5. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Div.; Univ. of California, Berkeley, CA (United States). Dept. of Physics
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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, few-femtosecond core-excited state lifetimes of iodine monochloride are obtained by 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 fs and 4.3 fs are obtained for core-hole states parallel to the bond and 6.5 fs and 6.9 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.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1633286
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 11; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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