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Journal Article

Ultrafast isomerization initiated by X-ray core ionization.


Boll,  R.
Research Group of Structural Dynamics of (Bio)Chemical Systems, MPI for Biophysical Chemistry, Max Planck Society;

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Liekhus-Schmaltz, C. E., Tenney, I., Osipov, T., Sanchez-Gonzalez, A., Berrah, N., Boll, R., et al. (2015). Ultrafast isomerization initiated by X-ray core ionization. Nature Communications, 6: 8199. doi:10.1038/ncomms9199.

Cite as: http://hdl.handle.net/11858/00-001M-0000-002C-017F-C
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.