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

Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis
Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis
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
1463-9076
22699-22709
Mcmanus, Joseph W.
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Walmsley, Tiffany
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Nagaya, Kiyonobu
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Harries, James R.
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Kumagai, Yoshiaki
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Iwayama, Hiroshi
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Ashfold, Michael N.R.
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Britton, Mathew
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Bucksbaum, Philip H.
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Downes-Ward, Briony
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Driver, Taran
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Heathcote, David
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Hockett, Paul
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Howard, Andrew J.
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Kukk, Edwin
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Lee, Jason W. L.
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Liu, Yusong
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Milesevic, Dennis
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Minns, Russell S.
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Niozu, Akinobu
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Niskanen, Johannes
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Orr-ewing, Andrew J.
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Owada, Shigeki
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Rolles, Daniel
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Robertson, Patrick A.
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Rudenko, Artem
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Ueda, Kiyoshi
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Unwin, James
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Vallance, Claire
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Burt, Michael
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Brouard, Mark
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Forbes, Ruaridh
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Allum, Felix
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Mcmanus, Joseph W.
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Walmsley, Tiffany
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Nagaya, Kiyonobu
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Harries, James R.
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Kumagai, Yoshiaki
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Iwayama, Hiroshi
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Ashfold, Michael N.R.
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Britton, Mathew
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Bucksbaum, Philip H.
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Downes-Ward, Briony
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Driver, Taran
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Heathcote, David
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Hockett, Paul
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Howard, Andrew J.
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Kukk, Edwin
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Lee, Jason W. L.
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Liu, Yusong
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Milesevic, Dennis
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Minns, Russell S.
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Niozu, Akinobu
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Niskanen, Johannes
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Owada, Shigeki
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Rolles, Daniel
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Rudenko, Artem
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Ueda, Kiyoshi
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Unwin, James
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Vallance, Claire
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Burt, Michael
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Brouard, Mark
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Forbes, Ruaridh
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Allum, Felix
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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 and Allum, Felix (2022) Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis. Physical Chemistry Chemical Physics, 24 (37), 22699-22709. (doi:10.1039/D2CP03029B).

Record type: Article

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

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Accepted/In Press date: 16 August 2022
e-pub ahead of print date: 15 September 2022
Published date: 28 September 2022
Additional Information: Funding Information: The experiment was performed at SACLA with the approval of JASRI and the program review committee (Proposal No. 2021A8038 Forbes). We thank the technical and scientific staff of SACLA for their hospitality and support before and during the beamtime. R. F. and F. A. gratefully acknowledge support from the Linac Coherent Light Source, SLAC National Accelerator Laboratory, which is supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under contract no. DE-AC02-76SF00515. D. R. and A. R. were supported by contract no. DE-FG02-86ER13491 from the same funding agency. J. W. L. L. acknowledges financial support via the Helmholtz-ERC Recognition Award (ERC-RA-0043) of the Helmholtz Association (HGF). B. D. W. thanks the CLF and the University of Southampton for a studentship. R. S. M. thanks the EPSRC for financial support (EP/R010609/1). J. M., M. Br., D. H., C. V. and A. J. O.-E. gratefully acknowledge the support of EPSRC Programme grant EP/V026690/1. P. A. R., C. V. and M. Br. also gratefully acknowledge the support of EPSRC Programme grant EP/T021675. M. Bu. and T. W. are grateful to EPSRC for support from EP/S028617/1. T. W. is additionally thankful to EPSRC for studentship funding and Jesus College, Oxford for a partial fee scholarship. P. H. B., A. J. H. and M. B. were supported by the National Science Foundation. A. J. H. was supported under a Stanford Graduate Fellowship as the 2019 Albion Walter Hewlett Fellow. Y. K. acknowledges support by JSPS KAKENHI Grant No. 20K14427. For the purpose of Open Access, the author has applied a CC BY public copyright licence to any Author Accepted Manuscript version arising from this submission. Publisher Copyright: © 2022 The Royal Society of Chemistry.
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Identifiers

Local EPrints ID: 469585
URI: http://eprints.soton.ac.uk/id/eprint/469585
DOI: doi:10.1039/D2CP03029B
ISSN: 1463-9076
PURE UUID: fd780c4f-f0a7-4a1b-ad13-ed09b3e12693
ORCID for Russell S. Minns: ORCID iD orcid.org/0000-0001-6775-2977

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Date deposited: 20 Sep 2022 16:56
Last modified: 06 Jun 2024 01:49

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Contributors

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

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