Ultrafast isomerization initiated by X-ray core ionization
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Liekhus-Schmaltz_Ultrafast isomerization.pdf
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705.6 KB
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4ebb12bd93383d9c433cd74c36053773
Author(s)
Field, Robert W.
Date Issued
September 2015
Journal
Nature Communications
Publisher
Nature Publishing Group
Citation
Liekhus-Schmaltz, Chelsea E., Ian Tenney, Timur Osipov, Alvaro Sanchez-Gonzalez, Nora Berrah, Rebecca Boll, Cedric Bomme, et al. “Ultrafast Isomerization Initiated by X-Ray Core Ionization.” Nat Comms 6 (September 10, 2015): 8199. © 2015 Macmillan Publishers Limited
Version
Final published version
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.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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DOI of Published Version
https://doi.org/10.1038/ncomms9199
