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Tuesday, 19 June 2012

Amelle: Conical Intersection Dynamics in NO2 Probed by Homodyne High-Harmonic Spectroscopy

Conical Intersection Dynamics in NO2 Probed by Homodyne High-Harmonic Spectroscopy
  1. D. M. Villeneuve1
+Author Affiliations
  1. 1Joint Laboratory for Attosecond Science, National Research Council of Canada and University of Ottawa, 100 Sussex Drive, Ottawa, Ontario, Canada K1A 0R6.
  2. 2Laboratorium für Physikalische Chemie, Eidgenössische Technische Hochschule Zürich, Wolfgang-Pauli-Strasse 10, 8093 Zürich, Switzerland.
  3. 3Centre Lasers Intenses et Applications, Université de Bordeaux, CEA, CNRS, UMR5107, 351 Cours de la Libération, 33405 Talence, France.
  4. 4Laboratoire Collisions Agrégats Réactivité (IRSAMC), UPS, Université de Toulouse, F-31062 Toulouse, France and CNRS, UMR 5589, F-31062 Toulouse, France
  1. *To whom correspondence should be addressed. E-mail:


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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