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We thank Dr. Alberto Garcia-Vela and Dr. Jesus Gonzalez Vazquez for fruitful discussions. M.E.C. acknowledges financial support from MICINN (Spain) through a FPU fellowship. This work has been financed by the Spanish MICINN through Grant No. CTQ2008-02578/BQU, the Consolider program "Science and Applications of Ultrafast Ultraintense Lasers," Grant No. CSD2007-00013, and by the European Union ITN network " Ultrafast control of quantum systems by strong laser fields-FASTQUAST" (Grant No. PITN-GA-2008-214962). This research has been performed within the Unidad Asociada "Quimica Fisica Molecular" between Departamento de Quimica Fisica of UCM and CSIC. The facilities provided by the Centro de Asistencia a la Investigacion de Espectroscopia Multifotonica y de Femtosegundo (UCM) are gratefully acknowledged.

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A femtosecond velocity map imaging study on B-band predissociation in CH3I. I. The band origin

Publicated to:JOURNAL OF CHEMICAL PHYSICS. 132 (23): 234313- - 2010-06-21 132(23), DOI: 10.1063/1.3455207

Authors: Gitzinger, G.; Corrales, M. E.; Loriot, V.; Amaral, G. A.; de Nalda, R.; Banares, L.;

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Abstract

A femtosecond pump-probe experiment, coupled with velocity map ion imaging, is reported on the second absorption band (B-band) of CH3I. The measurements provide a detailed picture of real-time B-band predissociation in the band origin at 201.2 nm. Several new data are reported. (i) A value of 1.5 +/- 0.1 ps has been obtained for the lifetime of the excited state, consistent within errors with the only other direct measurement of this quantity [A.P. Baronavski and J.C. Owrutsky, J. Chem. Phys. 108, 3445 (1998)]. (ii) It has been possible to measure the angular character of the transition directly through the observation of fragments appearing early with respect to both predissociation lifetime and molecular rotation. (iii) Vibrational activity in CH3 has been found, both in the umbrella (v(2)) and the symmetric stretch (v(1)) modes, with estimates of relative populations. All these findings constitute a challenge and a test for much-wanted high level ab initio and dynamics calculations in this energy region. (C) 2010 American Institute of Physics. [doi:10.1063/1.3455207]

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