title: Conical intersection dynamics in NO2 probed by homodyne high-harmonic spectroscopy.
abstract: Conical intersections play a crucial role in the chemistry of most polyatomic molecules, ranging from the simplest bimolecular reactions to the photostability of DNA. The real-time study of the associated electronic dynamics poses a major challenge to the latest techniques of ultrafast measurement. We show that high-harmonic spectroscopy reveals oscillations in the electronic character that occur in nitrogen dioxide when a photoexcited wave packet crosses a conical intersection. At longer delays, we observe the onset of statistical dissociation dynamics. The present results demonstrate that high-harmonic spectroscopy could become a powerful tool to highlight electronic dynamics occurring along nonadiabatic chemical reaction pathways.
authors: Joint Laboratory for Attosecond Science, National Research Council of Canada and University of Ottawa, Ottawa, Ontario, Canada. woerner@phys.chem.ethz.ch
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