Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 137, Issue 22, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.4768810
Keywords
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Funding
- ANR [ANR-08-JCJC-0029 HarMoDyn]
- Conseil Regional Aquitaine [20091304003 ATTOMOL, 2.1.3-09010502 COLA2]
- European Union through the MOLCOTUV
- European Union through the ITN-ICONIC
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We study theoretically and experimentally the electronic relaxation of NO2 molecules excited by absorption of one similar to 400 nm pump photon. Semiclassical simulations based on trajectory surface hopping calculations are performed. They predict fast oscillations of the electronic character around the intersection of the ground and first excited diabatic states. An experiment based on high-order harmonic transient grating spectroscopy reveals dynamics occurring on the same time scale. A systematic study of the detected transient is conducted to investigate the possible influence of the pump intensity, pump wavelength, and rotational temperature of the molecules. The quantitative agreement between measured and predicted dynamics shows that, in NO2, high harmonic transient grating spectroscopy encodes vibrational dynamics underlying the electronic relaxation. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4768810]
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