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12 pages, 6 figures, 4 tables.- PACS nrs: 33.20.Sn, 33.15.Mt, 33.20.Fb, 33.40.+f, 33.20.Tp, 33.80.Wz.A new technique for the direct determination of state-to-state rotational energy transfer rate constants in the gas phase is presented. It is based on two sequential stimulated Raman processes: the first one prepares the sample in a single rotational state of an excited vibrational level, and the second one, using the high resolution quasi-continuous stimulated Raman-loss technique, monitors the transfer of population to other rotational states of the same vibrational level as a function of the delay between the pump and the probe stages. The technique is applied to the odd-J rotational states of v2 = 1 acetylene at 155 K. The experimental layout, data acquisition, retrieval procedures, and numerical treatment are described. The quantity and quality of the data are high enough to allow a direct determination of the state-to-state rate constant matrix from a fit of the experimental data, with the only conditions of detailed balance and of a closed number of states. The matrix obtained from this direct fit is also compared with those obtained using some common fitting and scaling laws.This work has been funded by the Spanish Ministry of Education and Science through research Grant No. FIS2005-02029.Peer reviewe

the journal of chemical physics

Direct determination of state-to-state rotational energy transfer rate constants via a Raman-Raman double resonance technique: <i>ortho</i>-acetylene in v2=1 at 155 K

Direct determination of state-to-state rotational energy transfer rate constants via a Raman-Raman double resonance technique: ortho-acetylene in v2=1 at 155 K