A1 Refereed original research article in a scientific journal
Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis
Authors: McManus Joseph W., Walmsley Tiffany, Nagaya Kiyonobu, Harries James R., Kumagai Yoshiaki, Iwayama Hiroshi, Ashfold, Michael N. R., Britton Mathew, Bucksbaum Philip H., Downes-Ward Briony, Driver Taran, Heathcote David, Hockett Paul, Howard, Andrew J., Kukk Edwin, Lee Jason W. L., Liu Yusong, Milesevic Dennis, Minns Russell S., Niozu Akinobu, Niskanen Johannes, Orr-Ewing Andrew J., Owada Shigeki, Rolles Daniel, Robertson Patrick A., Rudenko Artem, Ueda Kiyoshi, Unwin James, Vallance Claire, Burt Michael, Brouard Mark, Forbes Ruaridh, Allum Felix
Publisher: The Royal Society of Chemistry
Publication year: 2022
Journal: Physical Chemistry Chemical Physics
Volume: 24
Issue: 37
First page : 22699
Last page: 22709
eISSN: 1463-9084
DOI: https://doi.org/10.1039/D2CP03029B
Web address : https://pubs.rsc.org/en/content/articlelanding/2022/cp/d2cp03029b
Self-archived copy’s web address: https://research.utu.fi/converis/portal/detail/Publication/176401164
We present results from an experimental ion imaging study into the fragmentation dynamics of 1-iodopropane and 2-iodopropane following interaction with extreme ultraviolet intense femtosecond laser pulses with a photon energy of 95 eV. Using covariance imaging analysis, a range of observed fragmentation pathways of the resulting polycations can be isolated and interrogated in detail at relatively high ion count rates (∼12 ions shot−1). By incorporating the recently developed native frames analysis approach into the three-dimensional covariance imaging procedure, contributions from three-body concerted and sequential fragmentation mechanisms can be isolated. The angular distribution of the fragment ions is much more complex than in previously reported studies for triatomic polycations, and differs substantially between the two isomeric species. With support of simple simulations of the dissociation channels of interest, detailed physical insights into the fragmentation dynamics are obtained, including how the initial dissociation step in a sequential mechanism influences rovibrational dynamics in the metastable intermediate ion and how signatures of this nuclear motion manifest in the measured signals.
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