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; Akinobo 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, 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, Akinobo NiozuJohannes 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

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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.

Original language	English
Pages (from-to)	22699-22709
Number of pages	11
Journal	Physical Chemistry Chemical Physics
Volume	24
Issue number	37
DOIs	https://doi.org/10.1039/D2CP03029B
Publication status	Published - 15 Sept 2022

Bibliographical note

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.

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© 2022 The Royal Society of Chemistry.

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10.1039/D2CP03029B

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Ultrafast Photochemical Dynamics in Gas and Condensed Phases
Orr-Ewing, A. J.
1/09/21 → 31/08/27
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McManus, J. W., Walmsley, T., Nagaya, K., Harries, J. R., Kumagai, Y., Iwayama, H., Ashfold, M. N. R., Britton, M., Bucksbaum, P. H., Downes-Ward, B., Driver, T., Heathcote, D., Hockett, P., Howard, A. J., Kukk, E., Lee, J. W. L., Liu, Y., Milesevic, D., Minns, R. S., ... Allum, F. (2022). Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis. Physical Chemistry Chemical Physics, 24(37), 22699-22709. https://doi.org/10.1039/D2CP03029B

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title = "Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis",

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.",

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

note = "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: {\textcopyright} 2022 The Royal Society of Chemistry.",

year = "2022",

month = sep,

day = "15",

doi = "10.1039/D2CP03029B",

language = "English",

volume = "24",

pages = "22699--22709",

journal = "Physical Chemistry Chemical Physics",

issn = "1463-9076",

publisher = "Royal Society of Chemistry",

number = "37",

}

McManus, JW, Walmsley, T, Nagaya, K, Harries, JR, Kumagai, Y, Iwayama, H, Ashfold, MNR, Britton, M, Bucksbaum, PH, Downes-Ward, B, Driver, T, Heathcote, D, Hockett, P, Howard, AJ, Kukk, E, Lee, JWL, Liu, Y, Milesevic, D, Minns, RS, Niozu, A, Niskanen, J, Orr-Ewing, AJ, Owada, S, Rolles, D, Robertson, PA, Rudenko, A, Ueda, K, Unwin, J, Vallance, C, Burt, M, Brouard, M, Forbes, R & Allum, F 2022, 'Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis', Physical Chemistry Chemical Physics, vol. 24, no. 37, pp. 22699-22709. https://doi.org/10.1039/D2CP03029B

TY - JOUR

T1 - Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis

AU - McManus, Joseph W

AU - Walmsley, Tiffany

AU - Nagaya, Kiyonobu

AU - Harries, James R

AU - Kumagai, Yoshiaki

AU - Iwayama, Hiroshi

AU - Ashfold, Michael N R

AU - Britton, Mathew

AU - Bucksbaum, Philip H

AU - Downes-Ward, Briony

AU - Driver, Taran

AU - Heathcote, David

AU - Hockett, Paul

AU - Howard, Andrew J

AU - Kukk, Edwin

AU - Lee, Jason W L

AU - Liu, Yusong

AU - Milesevic, Dennis

AU - Minns, Russell S

AU - Niozu, Akinobo

AU - Niskanen, Johannes

AU - Orr-Ewing, Andrew J

AU - Owada, Shigeki

AU - Rolles, Daniel

AU - Robertson, Patrick A

AU - Rudenko, Artem

AU - Ueda, Kiyoshi

AU - Unwin, James

AU - Vallance, Claire

AU - Burt, Michael

AU - Brouard, Mark

AU - Forbes, Ruaridh

AU - Allum, Felix

N1 - 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.

PY - 2022/9/15

Y1 - 2022/9/15

N2 - 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.

AB - 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.

U2 - 10.1039/D2CP03029B

DO - 10.1039/D2CP03029B

M3 - Article (Academic Journal)

C2 - 36106844

SN - 1463-9076

VL - 24

SP - 22699

EP - 22709

JO - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

IS - 37

ER -

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

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Ultrafast Photochemical Dynamics in Gas and Condensed Phases

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