Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis

Joseph W. McManus; Tiffany Walmsley; Kiyonobu Nagaya; James R. Harries; Yoshiaki Kumagai; Hiroshi Iwayama; Michael N.R. Ashfold; Mathew Britton; Philip H. Bucksbaum; Briony Downes-Ward; Taran Driver; David Heathcote; Paul Hockett; Andrew J. Howard; Edwin Kukk; Jason W. L. Lee; Yusong Liu; Dennis Milesevic; Russell S. Minns; Akinobu Niozu; Johannes Niskanen; Andrew J. Orr-Ewing; Shigeki Owada; Daniel Rolles; Patrick A. Robertson; Artem Rudenko; Kiyoshi Ueda; James Unwin; Claire Vallance; Michael Burt; Mark Brouard; Ruaridh Forbes; Felix Allum

doi:10.1039/D2CP03029B

Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis†

Joseph W. McManus,

‡^a Tiffany Walmsley,

‡^a Kiyonobu Nagaya,^b James R. Harries,^c Yoshiaki Kumagai,^d Hiroshi Iwayama,^e Michael N.R. Ashfold,

^f Mathew Britton,^g Philip H. Bucksbaum,^g Briony Downes-Ward,^h Taran Driver,

^g David Heathcote,

^a Paul Hockett,

ⁱ Andrew J. Howard,^g Edwin Kukk,^j Jason W. L. Lee,

^k Yusong Liu,

^g Dennis Milesevic,

^a Russell S. Minns,

^h Akinobu Niozu,

^l Johannes Niskanen,

^j Andrew J. Orr-Ewing,

^f Shigeki Owada,^mn Daniel Rolles,

^o Patrick A. Robertson,

^a Artem Rudenko,^o Kiyoshi Ueda,^p James Unwin,

^a Claire Vallance,

^a Michael Burt,

^a Mark Brouard,

^a Ruaridh Forbes

*^q and Felix Allum

*^agq

Author affiliations

* Corresponding authors

^a Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Oxford OX1 3TA, UK

^b Department of Physics, Kyoto University, Kyoto, Japan

^c QST, SPring-8, Kouto 1-1-1, Sayo, Hyogo, Japan

^d Department of Applied Physics, Tokyo University of Agriculture and Technology, Koganei-shi, Tokyo 184-8588, Japan

^e UVSOR Synchrotron Facility, Institute for Molecular Science, Okazaki 444-8585, Japan

^f School of Chemistry, University of Bristol, Cantock's Close, Bristol BS8 1TS, UK

^g Stanford PULSE Institute, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA

^h Chemistry, University of Southampton, Highfield, Southampton SO17 1BJ, UK

ⁱ National Research Council of Canada, 100 Sussex Dr., Ottawa, ON K1A 0R6, Canada

^j Department of Physics and Astronomy, University of Turku, Turku, Finland

^k Deutsches Elektronen-Synchrotron (DESY), Notkestraße 85, 22607 Hamburg, Germany

^l Graduate School of Advanced Science and Engineering, Hiroshima University, Higashi-Hiroshima 739-8526, Japan

^m RIKEN SPring-8 Center, Sayo, Hyogo, Japan

ⁿ Japan Synchrotron Radiation Research Institute, Hyogo, Japan

^o J. R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS, USA

^p Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai, Japan

^q Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA
E-mail: ruforbes@slac.stanford.edu, fallum@stanford.edu

Abstract

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.

This article is part of the themed collection: Ions, electrons, coincidences and dynamics: Festschrift for John H.D. Eland

Physical Chemistry Chemical Physics

Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis†

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Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis

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