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Conical intersection dynamics in NO2 probed by homodyne high-harmonic spectroscopy. 2011

H J Wörner, and J B Bertrand, and B Fabre, and J Higuet, and H Ruf, and A Dubrouil, and S Patchkovskii, and M Spanner, and Y Mairesse, and V Blanchet, and E Mével, and E Constant, and P B Corkum, and D M Villeneuve
Joint Laboratory for Attosecond Science, National Research Council of Canada and University of Ottawa, Ottawa, Ontario, Canada. woerner@phys.chem.ethz.ch

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.

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