Journal
SCIENCE
Volume 334, Issue 6053, Pages 208-212Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1208664
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Funding
- Swiss National Science Foundation [PP00P2_128274]
- Agence Nationale de la Recherche [ANR-08-JCJC-0029]
- Centre National de la Recherche Scientifique
- National Sciences and Engineering Research Council of Canada
- Canadian Institute for Photonic Innovations
- Air Force Office of Scientific Research
- Swiss National Science Foundation (SNF) [PP00P2_128274] Funding Source: Swiss National Science Foundation (SNF)
- Agence Nationale de la Recherche (ANR) [ANR-08-JCJC-0029] Funding Source: Agence Nationale de la Recherche (ANR)
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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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