Journal
NATURE PHYSICS
Volume 18, Issue 4, Pages 423-+Publisher
NATURE PORTFOLIO
DOI: 10.1038/s41567-022-01507-0
Keywords
-
Categories
Funding
- Deutsches Elektronen-Synchrotron (DESY)
Ask authors/readers for more resources
Intense femtosecond X-ray pulses can visualize the structural dynamics of exploding photoionized molecules, providing important insights into chemical reactions.
Visualizing the structural dynamics of isolated molecules would help to understand chemical reactions, but this is difficult for complex structures. Intense femtosecond X-ray pulses allow the full imaging of exploding photoionized molecules, in this case, with eleven atoms. Following structural dynamics in real time is a fundamental goal towards a better understanding of chemical reactions. Recording snapshots of individual molecules with ultrashort exposure times is a key ingredient towards this goal, as atoms move on femtosecond (10(-15) s) timescales. For condensed-phase samples, ultrafast, atomically resolved structure determination has been demonstrated using X-ray and electron diffraction. Pioneering experiments have also started addressing gaseous samples. However, they face the problem of low target densities, low scattering cross sections and random spatial orientation of the molecules. Therefore, obtaining images of entire, isolated molecules capturing all constituents, including hydrogen atoms, remains challenging. Here we demonstrate that intense femtosecond pulses from an X-ray free-electron laser trigger rapid and complete Coulomb explosions of 2-iodopyridine and 2-iodopyrazine molecules. We obtain intriguingly clear momentum images depicting ten or eleven atoms, including all the hydrogens, and thus overcome a so-far impregnable barrier for complete Coulomb explosion imaging-its limitation on molecules consisting of three to five atoms. In combination with state-of-the-art multi-coincidence techniques and elaborate theoretical modelling, this allows tracing ultrafast hydrogen emission and obtaining information on the result of intramolecular electron rearrangement. Our work represents an important step towards imaging femtosecond chemistry via Coulomb explosion.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available