期刊
NATURE COMMUNICATIONS
卷 6, 期 -, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms9199
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资金
- US Department of Energy Office of Science by Stanford University
- National Science Foundation [PHY-0649578]
- US Department of Energy, Office of Science, Basic Energy Sciences
- STFC
- EPSRC UK programme
- ERC ASTEX
- Max Planck Society
- Helmholtz Gemeinschaft through the Young Investigator Program
- LCLS, a DOE Office of Science User Facility
- Atomic and Molecular Optical Scisnces program within the Chemical Sciences, Geosciences, and Biosciences Division of the Office of Basic Energy Sciences, Office of Science, US Department of Energy
- Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, US Department of Energy
- EPSRC [EP/I032517/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [1227506, EP/I032517/1] Funding Source: researchfish
- Direct For Mathematical & Physical Scien
- Division Of Physics [0969322] Funding Source: National Science Foundation
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.
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