Published in
Nature Research, Nature Communications, 1(6), 2015
DOI: 10.1038/ncomms9199
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Ultrafast isomerization initiated by X-ray core ionization
,
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
and other authors.
Full text: Download
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.