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Originally published in Science Express on 15 December 2005
Science 13 January 2006:
Vol. 311. no. 5758, pp. 219 - 222
DOI: 10.1126/science.1120779
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Reports

Femtosecond Multidimensional Imaging of a Molecular Dissociation

O. Geßner,1 A. M. D. Lee,1,2 J. P. Shaffer,3 H. Reisler,4 S. V. Levchenko,4 A. I. Krylov,4 Jonathan G. Underwood,5 H. Shi,6 A. L. L. East,6 D. M. Wardlaw,2 E. t. H. Chrysostom,7 C. C. Hayden,7 Albert Stolow1,2*

The coupled electronic and vibrational motions governing chemical processes are best viewed from the molecule's point of view—the molecular frame. Measurements made in the laboratory frame often conceal information because of the random orientations the molecule can take. We used a combination of time-resolved photoelectron spectroscopy, multidimensional coincidence imaging spectroscopy, and ab initio computation to trace a complete reactant-to-product pathway—the photodissociation of the nitric oxide dimer—from the molecule's point of view, on the femtosecond time scale. This method revealed an elusive photochemical process involving intermediate electronic configurations.

1 Steacie Institute for Molecular Sciences, National Research Council Canada, Ottawa, Ontario K1A 0R6, Canada.
2 Department of Chemistry, Queen's University, Kingston, Ontario K7L 3N6, Canada.
3 Department of Physics and Astronomy, University of Oklahoma, Norman, OK 73019, USA.
4 Department of Chemistry, University of Southern California, Los Angeles, CA 90089, USA.
5 Department of Physics and Astronomy, Open University, Milton Keynes MK7 6AA, UK.
6 Department of Chemistry, University of Regina, Regina, Saskatchewan S4S 0A2, Canada.
7 Combustion Research Facility, Sandia National Laboratories, Livermore, CA 94551, USA.

* To whom correspondence should be addressed. E-mail: albert.stolow{at}nrc.ca

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