Imaging Molecular Motion: Femtosecond X-Ray Scattering of an Electrocyclic Chemical Reaction
Open accessAbstract
Structural rearrangements within single molecules occur on ultrafast time scales. Many aspects of molecular dynamics, such as the energy flow through excited states, have been studied using spectroscopic techniques, yet the goal to watch molecules evolve their geometrical structure in real time remains challenging. By mapping nuclear motions using femtosecond x-ray pulses, we have created real-space representations of the evolving dynamics during a well-known chemical reaction and show a series of time-sorted structural snapshots produced by ultrafast time-resolved hard x-ray scattering. A computational analysis optimally matches the series of scattering patterns produced by the x rays to a multitude of potential reaction paths. In so doing, we have made a critical step toward the goal of viewing chemical reactions on femtosecond time scales, opening a new direction in studies of ultrafast chemical reactions in the gas phase.
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X-ray diffraction experiments of isolated molecules in photoreaction have become feasible in the last few years, demonstrating that watching atomic motion in an isolated molecule is no longer a dream.
“X-ray diffraction experiments of isolated molecules in photoreaction have, however, become feasible in the last few years [10], demonstrating that watching atomic motion in an isolated molecule is no longer a dream.”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [10]
Rovibronic wavepackets in iodine, metal compounds in liquids and organic ring openings have all been observed with unprecedented time resolution.
“Rovibronic wavepackets in iodine, metal compounds in liquids and organic ring openings have all been observed with unprecedented time resolution [10,19,20].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [10]
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- Authors
- Minitti, M. P., Budarz, J. M., Kirrander, A., Robinson, J. S., Ratner, D., Lane, T. J., Zhu, D., Glownia, J. M., Kozina, M., Lemke, H. T., Sikorski, M., Feng, Y., Nelson, S., Saita, K., Stankus, B., Northey, T., Hastings, J. B., & Weber, P. M.
- Affiliations
- SLAC National Accelerator Laboratory (US)
- Brown University (US)
- University of Edinburgh (GB)
- ORCID
- Venue
- Physical Review Letters
- Publisher
- American Physical Society (APS)
- Published
- 2015-06-22
- Volume
- 114
- Issue
- 25
- Pages
- 255501-255501
- ISSN
- 0031-9007 (ISSN-L)
- 1079-7114
- OpenAlex
- W965729195
- Cited by
- 318
- References
- 40
- Citations by year
- 2026: 15 · 2025: 18 · 2024: 26 · 2023: 26 · 2022: 18 · 2021: 23 · 2020: 35 · 2019: 37 · 2018: 33 · 2017: 41 · 2016: 38 · 2015: 8
- FWCI
- 41.55
- Type
- journal article
- Language
- en
- Open access
- bronze
- doi.org
- Licence
- Locations
- Physical Review Letters (publishedVersion)
- PubMed (publishedVersion)
- Edinburgh Research Explorer (University of Edinburgh) (submittedVersion, other-oa)
- Funders
- National Science Foundation (CBET-1336105)
- Seventh Framework Programme (FP7-PEOPLE-2013-CIG-NEWLIGHT)
- Leverhulme Trust (RPG-2013-365)
- Topics
- Physical Sciences › Physics and Astronomy › Radiation › Advanced X-ray Imaging Techniques
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
- Physical Sciences › Physics and Astronomy › Radiation › X-ray Spectroscopy and Fluorescence Analysis
- Keywords
- electrocyclic reactions, ultrafast chemical reactions, molecular dynamics, nuclear motion, gas-phase reactions
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