Native Frames: Disentangling Sequential from Concerted Three-Body Fragmentation

Jyoti Rajput, T. Severt, Ben Berry, Bethany Jochim, Peyman Feizollah, Balram Kaderiya, M. Zohrabi, U. Ablikim, Farzaneh Ziaee, Kanaka Raju P., D. Rolles, A. Rudenko, K. D. Carnes, B. D. Esry, and I. Ben-Itzhak
Phys. Rev. Lett. 120, 103001 – Published 8 March 2018

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.

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  • Received 18 November 2017

DOI:https://doi.org/10.1103/PhysRevLett.120.103001

© 2018 American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & Optical

Authors & Affiliations

Jyoti Rajput*, T. Severt, Ben Berry, Bethany Jochim, Peyman Feizollah, Balram Kaderiya, M. Zohrabi, U. Ablikim, Farzaneh Ziaee, Kanaka Raju P., D. Rolles, A. Rudenko, K. D. Carnes, B. D. Esry, and I. Ben-Itzhak

  • J. R. Macdonald Laboratory, Physics Department, Kansas State University, Manhattan, Kansas 66506, USA

  • *Present address: Department of Physics and Astrophysics, University of Delhi, Delhi 110007, India.
  • ibi@phys.ksu.edu

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Issue

Vol. 120, Iss. 10 — 9 March 2018

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