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

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.

SUBMITTER: Marroux HJB 

PROVIDER: S-EPMC7669856 | biostudies-literature | 2020 Nov

REPOSITORIES: biostudies-literature