Ultrafast isomerization initiated by X-ray core ionization

Liekhus-Schmaltz, Chelsea E.; Tenney, Ian; Osipov, Timur; Sanchez-Gonzalez, Alvaro; Berrah, Nora; Boll, Rebecca; Bomme, Cedric; Bostedt, Christoph; Bozek, John D.; Carron, Sebastian; Coffee, Ryan; Devin, Julien; Erk, Benjamin; Ferguson, Ken R.; Field, Robert W.; Foucar, Lutz; Frasinski, Leszek J.; Glownia, James M.; Gühr, Markus; Kamalov, Andrei; Krzywinski, Jacek; Li, Heng; Marangos, Jonathan P.; Martinez, Todd J.; McFarland, Brian K.; Miyabe, Shungo; Murphy, Brendan; Natan, Adi; Rolles, Daniel; Rudenko, Artem; Siano, Marco; Simpson, Emma R.; Spector, Limor; Swiggers, Michele; Walke, Daniel; Wang, Song; Weber, Thorsten; Bucksbaum, Philip H.; Petrovic, Vladimir S.

doi:10.1038/ncomms9199

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Ultrafast isomerization initiated by X-ray core ionization

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Foucar, Lutz
Department of Biomolecular Mechanisms, Max Planck Institute for Medical Research, Max Planck Society;

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http://www.nature.com/ncomms/2015/150910/ncomms9199/pdf/ncomms9199.pdf
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https://dx.doi.org/10.1038/ncomms9199
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引用

Liekhus-Schmaltz, C. E., Tenney, I., Osipov, T., Sanchez-Gonzalez, A., Berrah, N., Boll, R., Bomme, C., Bostedt, C., Bozek, J. D., Carron, S., Coffee, R., Devin, J., Erk, B., Ferguson, K. R., Field, R. W., Foucar, L., Frasinski, L. J., Glownia, J. M., Gühr, M., Kamalov, A., Krzywinski, J., Li, H., Marangos, J. P., Martinez, T. J., McFarland, B. K., Miyabe, S., Murphy, B., Natan, A., Rolles, D., Rudenko, A., Siano, M., Simpson, E. R., Spector, L., Swiggers, M., Walke, D., Wang, S., Weber, T., Bucksbaum, P. H., & Petrovic, V. S. (2015). Ultrafast isomerization initiated by X-ray core ionization. Nature Communications, 6:, pp. 1-7. doi:10.1038/ncomms9199.

引用: https://hdl.handle.net/11858/00-001M-0000-002A-212A-C

要旨

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.