Native Frames: Disentangling Sequential from Concerted Three-Body Fragmentation

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dc.contributor.author Rajput, Jyoti
dc.contributor.author Severt, T.
dc.contributor.author Berry, Ben
dc.contributor.author Jochim, Bethany
dc.contributor.author Feizollah, Peyman
dc.contributor.author Kaderiya, Balram
dc.contributor.author Zohrabi, M.
dc.contributor.author Ablikim, U.
dc.contributor.author Ziaee, Farzaneh
dc.contributor.author Raju P., Kanaka
dc.contributor.author Rolles, D.
dc.contributor.author Rudenko, A.
dc.contributor.author Carnes, K. D.
dc.contributor.author Esry, B. D.
dc.contributor.author Ben-Itzhak, I.
dc.date.accessioned 2019-04-17T14:12:56Z
dc.date.available 2019-04-17T14:12:56Z
dc.date.issued 2018-03-08
dc.identifier.uri http://hdl.handle.net/2097/39536
dc.description Citation: Rajput, J., Severt, T., Berry, B., Jochim, B., Feizollah, P., Kaderiya, B., … Ben-Itzhak, I. (2018). Native Frames: Disentangling Sequential from Concerted Three-Body Fragmentation. Physical Review Letters, 120(10), 103001. https://doi.org/10.1103/PhysRevLett.120.103001
dc.description.abstract A key question concerning the three-body fragmentation of polyatomic molecules is the distinction of sequential and concerted mechanisms, i.e., the stepwise or simultaneous cleavage of bonds. Using laser-driven fragmentation of OCS into O++C++S+ and employing coincidence momentum imaging, we demonstrate a novel method that enables the clear separation of sequential and concerted breakup. The separation is accomplished by analyzing the three-body fragmentation in the native frame associated with each step and taking advantage of the rotation of the intermediate molecular fragment, CO2+ or CS2+, before its unimolecular dissociation. This native-frame method works for any projectile (electrons, ions, or photons), provides details on each step of the sequential breakup, and enables the retrieval of the relevant spectra for sequential and concerted breakup separately. Specifically, this allows the determination of the branching ratio of all these processes in OCS3+ breakup. Moreover, we find that the first step of sequential breakup is tightly aligned along the laser polarization and identify the likely electronic states of the intermediate dication that undergo unimolecular dissociation in the second step. Finally, the separated concerted breakup spectra show clearly that the central carbon atom is preferentially ejected perpendicular to the laser field.
dc.language.iso en_US
dc.relation.uri https://doi.org/10.1103/PhysRevLett.120.103001
dc.rights © 2018 American Physical Society
dc.rights.uri https://journals.aps.org/authors/transfer-of-copyright-agreement
dc.rights.uri https://rightsstatements.org/page/InC/1.0/?language=en
dc.subject Light-matter interaction
dc.subject Multiphoton or tunneling ionization & excitation
dc.subject Photodissociation
dc.subject Single- and few-photon ionization & excitation
dc.title Native Frames: Disentangling Sequential from Concerted Three-Body Fragmentation
dc.type Text
dc.date.published 2018
dc.citation.doi 10.1103/PhysRevLett.120.103001
dc.citation.issn 1079-7114
dc.citation.issue 10
dc.citation.jtitle Physical Review Letters
dc.citation.volume 120
dc.citation Rajput, J., Severt, T., Berry, B., Jochim, B., Feizollah, P., Kaderiya, B., … Ben-Itzhak, I. (2018). Native Frames: Disentangling Sequential from Concerted Three-Body Fragmentation. Physical Review Letters, 120(10), 103001. https://doi.org/10.1103/PhysRevLett.120.103001
dc.description.version Article: Version of Record (VoR)


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