期刊
JOURNAL OF CHEMICAL PHYSICS
卷 135, 期 5, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.3615544
关键词
dark states; high-speed optical techniques; molecular electronic states; nonradiative transitions; organic compounds; photoexcitation; photoionisation
资金
- Spanish MICINN [CTQ2010-17749]
- Consolider Program Science and Applications of Ultrafast Ultraintense Lasers [CSD2007-00013]
The ultrafast relaxation of jet-cooled aniline was followed by time-resolved ionization, after excitation in the 294-234 interval. The studied range of energy covers the absorption of the two bright pi pi* excitations, S-1 and S-3, and the almost dark S-2 (pi sigma*) state. The employed probe wavelengths permit to identify different ultrafast time constants related with the coupling of the involved electronic surfaces. A tau(1) = 165 +/- 30 fs lifetime is attributed to dynamics along the S-2 (pi sigma*) repulsive surface. Other relaxation channels as the S-1 -> S-0 and S-3 -> S-1 internal conversion are also identified and characterized. The work provides a general view of the photophysics of aniline, particularly regarding the role of the pi sigma* state. This state appears as minor dissipation process due to the ineffective coupling with the bright S-1 and S-3 states, being the S-1 -> S-0 internal conversion the main non-radiative process in the full studied energy range. Additionally, the influence of the off-resonance adiabatic excitation of higher energy electronic states, particularly S-3, is also observed and discussed. (C) 2011 American Institute of Physics. [doi:10.1063/1.3615544]
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