- H. J. Wörner1,2,*,
- J. B. Bertrand1,
- B. Fabre3,
- J. Higuet3,
- H. Ruf3,
- A. Dubrouil3,
- S. Patchkovskii1,
- M. Spanner1,
- Y. Mairesse3,
- V. Blanchet4,
- E. Mével3,
- E. Constant3,
- P. B. Corkum1,
- D. M. Villeneuve1
+Author Affiliations
- ↵*To whom correspondence should be addressed. E-mail: woerner@phys.chem.ethz.ch
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.
http://www.sciencemag.org/content/334/6053/208
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