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Time-resolved relaxation and fragmentation of polycyclic aromatic hydrocarbons investigated in the ultrafast XUV-IR regime

Author

Listed:
  • J. W. L. Lee

    (Deutsches Elektronen-Synchrotron DESY
    University of Oxford)

  • D. S. Tikhonov

    (Deutsches Elektronen-Synchrotron DESY
    Christian-Albrechts-Universität zu Kiel)

  • P. Chopra

    (Deutsches Elektronen-Synchrotron DESY
    Christian-Albrechts-Universität zu Kiel)

  • S. Maclot

    (Lund University
    University of Gothenburg)

  • A. L. Steber

    (Deutsches Elektronen-Synchrotron DESY
    Christian-Albrechts-Universität zu Kiel
    Universität Hamburg)

  • S. Gruet

    (Deutsches Elektronen-Synchrotron DESY)

  • F. Allum

    (University of Oxford)

  • R. Boll

    (European XFEL)

  • X. Cheng

    (Deutsches Elektronen-Synchrotron DESY)

  • S. Düsterer

    (Deutsches Elektronen-Synchrotron DESY)

  • B. Erk

    (Deutsches Elektronen-Synchrotron DESY)

  • D. Garg

    (Deutsches Elektronen-Synchrotron DESY
    Universität Hamburg)

  • L. He

    (Deutsches Elektronen-Synchrotron DESY)

  • D. Heathcote

    (University of Oxford)

  • M. Johny

    (Deutsches Elektronen-Synchrotron DESY)

  • M. M. Kazemi

    (Deutsches Elektronen-Synchrotron DESY)

  • H. Köckert

    (University of Oxford)

  • J. Lahl

    (Lund University)

  • A. K. Lemmens

    (FELIX Laboratory
    University of Amsterdam)

  • D. Loru

    (Deutsches Elektronen-Synchrotron DESY
    Christian-Albrechts-Universität zu Kiel)

  • R. Mason

    (University of Oxford)

  • E. Müller

    (Deutsches Elektronen-Synchrotron DESY)

  • T. Mullins

    (Deutsches Elektronen-Synchrotron DESY)

  • P. Olshin

    (Saint Petersburg State University)

  • C. Passow

    (Deutsches Elektronen-Synchrotron DESY)

  • J. Peschel

    (Lund University)

  • D. Ramm

    (Deutsches Elektronen-Synchrotron DESY)

  • D. Rompotis

    (Deutsches Elektronen-Synchrotron DESY
    European XFEL)

  • N. Schirmel

    (Deutsches Elektronen-Synchrotron DESY)

  • S. Trippel

    (Universität Hamburg
    Deutsches Elektronen-Synchrotron DESY)

  • J. Wiese

    (Deutsches Elektronen-Synchrotron DESY
    Universität Hamburg)

  • F. Ziaee

    (Kansas State University)

  • S. Bari

    (Deutsches Elektronen-Synchrotron DESY)

  • M. Burt

    (University of Oxford)

  • J. Küpper

    (Universität Hamburg
    Universität Hamburg
    Deutsches Elektronen-Synchrotron DESY
    Universität Hamburg)

  • A. M. Rijs

    (FELIX Laboratory
    Vrije Universiteit Amsterdam)

  • D. Rolles

    (Kansas State University)

  • S. Techert

    (Deutsches Elektronen-Synchrotron DESY
    Georg-August-Universität)

  • P. Eng-Johnsson

    (Lund University)

  • M. Brouard

    (University of Oxford)

  • C. Vallance

    (University of Oxford)

  • B. Manschwetus

    (Deutsches Elektronen-Synchrotron DESY)

  • M. Schnell

    (Deutsches Elektronen-Synchrotron DESY
    Christian-Albrechts-Universität zu Kiel)

Abstract

Polycyclic aromatic hydrocarbons (PAHs) play an important role in interstellar chemistry and are subject to high energy photons that can induce excitation, ionization, and fragmentation. Previous studies have demonstrated electronic relaxation of parent PAH monocations over 10–100 femtoseconds as a result of beyond-Born-Oppenheimer coupling between the electronic and nuclear dynamics. Here, we investigate three PAH molecules: fluorene, phenanthrene, and pyrene, using ultrafast XUV and IR laser pulses. Simultaneous measurements of the ion yields, ion momenta, and electron momenta as a function of laser pulse delay allow a detailed insight into the various molecular processes. We report relaxation times for the electronically excited PAH*, PAH+* and PAH2+* states, and show the time-dependent conversion between fragmentation pathways. Additionally, using recoil-frame covariance analysis between ion images, we demonstrate that the dissociation of the PAH2+ ions favors reaction pathways involving two-body breakup and/or loss of neutral fragments totaling an even number of carbon atoms.

Suggested Citation

  • J. W. L. Lee & D. S. Tikhonov & P. Chopra & S. Maclot & A. L. Steber & S. Gruet & F. Allum & R. Boll & X. Cheng & S. Düsterer & B. Erk & D. Garg & L. He & D. Heathcote & M. Johny & M. M. Kazemi & H. K, 2021. "Time-resolved relaxation and fragmentation of polycyclic aromatic hydrocarbons investigated in the ultrafast XUV-IR regime," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-26193-z
    DOI: 10.1038/s41467-021-26193-z
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    References listed on IDEAS

    as
    1. Theodore P. Snow & Valery Le Page & Yeghis Keheyan & Veronica M. Bierbaum, 1998. "The interstellar chemistry of PAH cations," Nature, Nature, vol. 391(6664), pages 259-260, January.
    2. A. Marciniak & V. Despré & T. Barillot & A. Rouzée & M.C.E. Galbraith & J. Klei & C.-H. Yang & C.T.L. Smeenk & V. Loriot & S. Nagaprasad Reddy & A.G.G.M. Tielens & S. Mahapatra & A. I. Kuleff & M.J.J., 2015. "XUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment," Nature Communications, Nature, vol. 6(1), pages 1-6, November.
    Full references (including those not matched with items on IDEAS)

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