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 fragmenta...
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| Published in | Physical chemistry chemical physics : PCCP Vol. 24; no. 37; pp. 22699 - 2279 |
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| Main Authors | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Cambridge
Royal Society of Chemistry
28.09.2022
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| Subjects | |
| Online Access | Get full text |
| ISSN | 1463-9076 1463-9084 1463-9084 |
| DOI | 10.1039/D2CP03029B |
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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. NRC publication: Yes |
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| AbstractList | 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. 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. 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.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. 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. Using covariance analysis methods, we study the fragmentation dynamics of multiply ionized 1- and 2-iodopropane. Signatures of isomer-specific nuclear motion occurring during sequential fragmentation pathways are identified. 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. 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 | Harries, James R Downes-Ward, Briony Rudenko, Artem Britton, Mathew Kumagai, Yoshiaki Hockett, Paul Lee, Jason W. L Vallance, Claire Owada, Shigeki Ashfold, Michael N.R Bucksbaum, Philip H Milesevic, Dennis Allum, Felix Robertson, Patrick A Nagaya, Kiyonobu Brouard, Mark Niozu, Akinobu McManus, Joseph W Walmsley, Tiffany Driver, Taran Minns, Russell S Unwin, James Forbes, Ruaridh Heathcote, David Kukk, Edwin Burt, Michael Niskanen, Johannes Rolles, Daniel Iwayama, Hiroshi Liu, Yusong Howard, Andrew J Orr-Ewing, Andrew J Ueda, Kiyoshi |
| AuthorAffiliation | QST, SPring-8 Department of Physics and Astronomy, University of Turku Chemistry, University of Southampton Department of Physics, Kyoto University J. R. Macdonald Laboratory, Department of Physics, Kansas State University Institute of Multidisciplinary Research for Advanced Materials, Tohoku University Deutsches Elektronen-Synchrotron (DESY) Linac Coherent Light Source, SLAC National Accelerator Laboratory Japan Synchrotron Radiation Research Institute School of Chemistry, University of Bristol, Cantock's Close Stanford PULSE Institute, SLAC National Accelerator Laboratory Chemistry Research Laboratory, Department of Chemistry, University of Oxford UVSOR Synchrotron Facility, Institute for Molecular Science RIKEN SPring-8 Center National Research Council of Canada Department of Applied Physics, Tokyo University of Agriculture and Technology, Koganei-shi, Tokyo 184-8588 Graduate School of Advanced Science and Engineering, Hiroshima University |
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| Author_xml | – sequence: 1 fullname: McManus, Joseph W – sequence: 2 fullname: Walmsley, Tiffany – sequence: 3 fullname: Nagaya, Kiyonobu – sequence: 4 fullname: Harries, James R – sequence: 5 fullname: Kumagai, Yoshiaki – sequence: 6 fullname: Iwayama, Hiroshi – sequence: 7 fullname: Ashfold, Michael N.R – sequence: 8 fullname: Britton, Mathew – sequence: 9 fullname: Bucksbaum, Philip H – sequence: 10 fullname: Downes-Ward, Briony – sequence: 11 fullname: Driver, Taran – sequence: 12 fullname: Heathcote, David – sequence: 13 fullname: Hockett, Paul – sequence: 14 fullname: Howard, Andrew J – sequence: 15 fullname: Kukk, Edwin – sequence: 16 fullname: Lee, Jason W. L – sequence: 17 fullname: Liu, Yusong – sequence: 18 fullname: Milesevic, Dennis – sequence: 19 fullname: Minns, Russell S – sequence: 20 fullname: Niozu, Akinobu – sequence: 21 fullname: Niskanen, Johannes – sequence: 22 fullname: Orr-Ewing, Andrew J – sequence: 23 fullname: Owada, Shigeki – sequence: 24 fullname: Rolles, Daniel – sequence: 25 fullname: Robertson, Patrick A – sequence: 26 fullname: Rudenko, Artem – sequence: 27 fullname: Ueda, Kiyoshi – sequence: 28 fullname: Unwin, James – sequence: 29 fullname: Vallance, Claire – sequence: 30 fullname: Burt, Michael – sequence: 31 fullname: Brouard, Mark – sequence: 32 fullname: Forbes, Ruaridh – sequence: 33 fullname: Allum, Felix |
| BackLink | https://www.osti.gov/biblio/1887595$$D View this record in Osti.gov |
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| SubjectTerms | Angular distribution Covariance Femtosecond pulses Fragmentation Imaging INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Polyelectrolytes |
| Title | Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis |
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