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Ultrafast isomerization initiated by X-ray core ionization

Author

Listed:
  • Chelsea E. Liekhus-Schmaltz

    (Stanford University
    PULSE Institute for Ultrafast Energy Science)

  • Ian Tenney

    (Stanford University
    PULSE Institute for Ultrafast Energy Science)

  • Timur Osipov

    (University of Connecticut)

  • Alvaro Sanchez-Gonzalez

    (Imperial College London)

  • Nora Berrah

    (University of Connecticut)

  • Rebecca Boll

    (Deutsches Elektronen-Synchrotron
    Max Planck Institute for Nuclear Physics)

  • Cedric Bomme

    (Deutsches Elektronen-Synchrotron)

  • Christoph Bostedt

    (Linac Coherent Light Source)

  • John D. Bozek

    (Linac Coherent Light Source)

  • Sebastian Carron

    (Linac Coherent Light Source)

  • Ryan Coffee

    (Linac Coherent Light Source)

  • Julien Devin

    (Stanford University
    PULSE Institute for Ultrafast Energy Science)

  • Benjamin Erk

    (Deutsches Elektronen-Synchrotron)

  • Ken R. Ferguson

    (Linac Coherent Light Source
    Stanford University)

  • Robert W. Field

    (Massachusetts Institute of Technology)

  • Lutz Foucar

    (Max Planck Institute for Medical Research)

  • Leszek J. Frasinski

    (Imperial College London)

  • James M. Glownia

    (Linac Coherent Light Source)

  • Markus Gühr

    (PULSE Institute for Ultrafast Energy Science)

  • Andrei Kamalov

    (Stanford University
    PULSE Institute for Ultrafast Energy Science)

  • Jacek Krzywinski

    (Linac Coherent Light Source)

  • Heng Li

    (PULSE Institute for Ultrafast Energy Science
    Linac Coherent Light Source)

  • Jonathan P. Marangos

    (Imperial College London)

  • Todd J. Martinez

    (PULSE Institute for Ultrafast Energy Science
    Stanford University)

  • Brian K. McFarland

    (PULSE Institute for Ultrafast Energy Science)

  • Shungo Miyabe

    (PULSE Institute for Ultrafast Energy Science
    Stanford University)

  • Brendan Murphy

    (University of Connecticut)

  • Adi Natan

    (PULSE Institute for Ultrafast Energy Science)

  • Daniel Rolles

    (Deutsches Elektronen-Synchrotron)

  • Artem Rudenko

    (J. R. Macdonald Laboratory, Kansas State University)

  • Marco Siano

    (Imperial College London)

  • Emma R. Simpson

    (Imperial College London)

  • Limor Spector

    (Stanford University
    PULSE Institute for Ultrafast Energy Science)

  • Michele Swiggers

    (Linac Coherent Light Source)

  • Daniel Walke

    (Imperial College London)

  • Song Wang

    (Stanford University
    PULSE Institute for Ultrafast Energy Science)

  • Thorsten Weber

    (Lawrence Berkeley National Lab)

  • Philip H. Bucksbaum

    (Stanford University
    PULSE Institute for Ultrafast Energy Science
    Stanford University)

  • Vladimir S. Petrovic

    (Stanford University
    PULSE Institute for Ultrafast Energy Science)

Abstract

Rapid proton migration is a key process in hydrocarbon photochemistry. Charge migration and subsequent proton motion can mitigate radiation damage when heavier atoms absorb X-rays. If rapid enough, this can improve the fidelity of diffract-before-destroy measurements of biomolecular structure at X-ray-free electron lasers. Here we study X-ray-initiated isomerization of acetylene, a model for proton dynamics in hydrocarbons. Our time-resolved measurements capture the transient motion of protons following X-ray ionization of carbon K-shell electrons. We Coulomb-explode the molecule with a second precisely delayed X-ray pulse and then record all the fragment momenta. These snapshots at different delays are combined into a ‘molecular movie’ of the evolving molecule, which shows substantial proton redistribution within the first 12 fs. We conclude that significant proton motion occurs on a timescale comparable to the Auger relaxation that refills the K-shell vacancy.

Suggested Citation

  • Chelsea E. Liekhus-Schmaltz & Ian Tenney & Timur Osipov & Alvaro Sanchez-Gonzalez & Nora Berrah & Rebecca Boll & Cedric Bomme & Christoph Bostedt & John D. Bozek & Sebastian Carron & Ryan Coffee & Jul, 2015. "Ultrafast isomerization initiated by X-ray core ionization," Nature Communications, Nature, vol. 6(1), pages 1-7, November.
    • Handle: RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms9199
    DOI: 10.1038/ncomms9199
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