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Published Online December 15, 2005
Science DOI: 10.1126/science.1120779

Reports

Submitted on September 30, 2005
Accepted on November 28, 2005

Femtosecond Multidimensional Imaging of a Molecular Dissociation

Oliver Gessner 1, A. M. D. Lee 2, James P. Shaffer 3, Hanna Reisler 4, Sergey V. Levchenko 4, Anna I. Krylov 4, Jonathan G. Underwood 5, H. Shi 6, Allan L. L. East 6, D. M. Wardlaw 7, Ester t. H. Chrysostom 8, Carl C. Hayden 8, Albert Stolow 2*

1 Steacie Institute for Molecular Sciences, National Research Council Canada, Ottawa, Ontario K1A 0R6, Canada.
2 Steacie Institute for Molecular Sciences, National Research Council Canada, Ottawa, Ontario K1A 0R6, Canada; 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 Department of Chemistry, Queen's University, Kingston, Ontario K7L 3N6, Canada.
8 Combustion Research Facility, Sandia National Laboratories, Livermore, CA 94551, USA.

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

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 lab frame often conceal information due to the random orientations the molecule can take. Here we trace a complete reactant-to-product pathway, from the molecule's point of view, on the femtosecond timescale using a combination of time-resolved photoelectron spectroscopy, multidimensional coincidence imaging spectroscopy and ab initio computation. We study the photodissociation of the nitric oxide dimer, unveiling an elusive process involving intermediate electronic configurations which was until now obscure.


THIS ARTICLE HAS BEEN CITED BY OTHER ARTICLES:
Time-Resolved Molecular Frame Dynamics of Fixed-in-Space CS2 Molecules.
C. Z. Bisgaard, O. J. Clarkin, G. Wu, A. M. D. Lee, O. Gessner, C. C. Hayden, and A. Stolow (2009)
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Time-Resolved Dynamics in N2O4 Probed Using High Harmonic Generation.
W. Li, X. Zhou, R. Lock, S. Patchkovskii, A. Stolow, H. C. Kapteyn, and M. M. Murnane (2008)
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Soft X-ray-Driven Femtosecond Molecular Dynamics.
E. Gagnon, P. Ranitovic, X.-M. Tong, C. L. Cocke, M. M. Murnane, H. C. Kapteyn, and A. S. Sandhu (2007)
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An electronic time scale in chemistry.
F. Remacle and R. D. Levine (2006)
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Science. ISSN 0036-8075 (print), 1095-9203 (online)