Ultrafast isomerization initiated by X-ray core ionization

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, Julien Devin, Benjamin Erk, Ken R. Ferguson, Robert W. Field, Lutz Foucar, Leszek J. Frasinski, James M. Glownia, Markus Gühr, Andrei Kamalov, Jacek Krzywinski, Heng Li, Jonathan P. Marangos, Todd J. Martinez, Brian K. McFarland, Shungo Miyabe, Brendan Murphy, Adi Natan, Daniel Rolles, Artem Rudenko, Marco Siano, Emma R. Simpson, Limor Spector, Michele Swiggers, Daniel Walke, Song Wang, Thorsten Weber, Philip H. Bucksbaum and Vladimir S. Petrovic ()
Additional contact information
Chelsea E. Liekhus-Schmaltz: Stanford University
Ian Tenney: Stanford University
Timur Osipov: University of Connecticut
Alvaro Sanchez-Gonzalez: Imperial College London
Nora Berrah: University of Connecticut
Rebecca Boll: Deutsches Elektronen-Synchrotron
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
Benjamin Erk: Deutsches Elektronen-Synchrotron
Ken R. Ferguson: Linac Coherent Light Source
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
Jacek Krzywinski: Linac Coherent Light Source
Heng Li: PULSE Institute for Ultrafast Energy Science
Jonathan P. Marangos: Imperial College London
Todd J. Martinez: PULSE Institute for Ultrafast Energy Science
Brian K. McFarland: PULSE Institute for Ultrafast Energy Science
Shungo Miyabe: PULSE Institute for Ultrafast Energy Science
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
Michele Swiggers: Linac Coherent Light Source
Daniel Walke: Imperial College London
Song Wang: Stanford University
Thorsten Weber: Lawrence Berkeley National Lab
Philip H. Bucksbaum: Stanford University
Vladimir S. Petrovic: Stanford University

Nature Communications, 2015, vol. 6, issue 1, 1-7

Abstract: 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.

Date: 2015
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DOI: 10.1038/ncomms9199

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