High-harmonic transient grating spectroscopy of NO2 electronic relaxation

التفاصيل البيبلوغرافية
العنوان: High-harmonic transient grating spectroscopy of NO2 electronic relaxation
المؤلفون: Ruf, H., Handschin, C., Ferré, A., Thiré, N., Bertrand, J. B., Bonnet, L., Cireasa, R., Constant, E., Corkum, P. B., Descamps, D., Fabre, B., Larregaray, P., Mével, E., Petit, S., Pons, B., Staedter, D., Wörner, H. J., Villeneuve, D. M., Mairesse, Y., Halvick, P., Blanchet, V.
سنة النشر: 2012
المجموعة: Physics (Other)
مصطلحات موضوعية: Physics - Chemical Physics, Physics - Atomic Physics, Physics - Optics
الوصف: We study theoretically and experimentally the electronic relaxation of NO2 molecules excited by absorption of one ~400 nm pump photon. Semi-classical 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 occuring on the same timescale. 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.
Comment: The following article has been accepted by Journal of Chemical Physics. After it is published, it will be found at http://jcp.aip.org/
نوع الوثيقة: Working Paper
DOI: 10.1063/1.4768810
URL الوصول: http://arxiv.org/abs/1211.0917
رقم الأكسشن: edsarx.1211.0917
قاعدة البيانات: arXiv