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Phys Rev Lett. 2015 Jun 26;114(25):255501. Epub 2015 Jun 22.

Imaging Molecular Motion: Femtosecond X-Ray Scattering of an Electrocyclic Chemical Reaction.

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SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA.
Brown University, Department of Chemistry, Providence, Rhode Island 02912, USA.
School of Chemistry, University of Edinburgh, Edinburgh EH9 3FJ, United Kingdom.
Stanford University, Department of Chemistry, Stanford, California 94305, USA.


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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