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VOLUME 93 (2011) | ISSUE 3 | PAGE 139
Extremely slow intramolecular vibrational redistribution: Direct observation by time- resolved Raman spectroscopy in trifluoropropyne
Abstract
We have studied the dynamics of intramolecular vibrational redistribution (IVR) from the initially excited mode \nu_1\approx3330 cm-1 (acetylene- type H-C bond) in H- C\equivC-CF3 molecules in the gaseous phase by means of anti- Stokes spontaneous Raman scattering. The time constant of this process is estimated as 2.3 ns- this is the slowest IVR time reported so far for the room-temperature gases. It is suggested that so long IVR time with respect to the other propyne derivatives can be explained by a larger defect, in this case, of the Fermi resonance of ν1 with ν2+2ν7- the most probable doorway state leading to IVR from ν1 to the bath of all vibrational-rotational states with the close energies. In addition, it is shown that the observed dynamics is in agreement with a theoretical model assuming strong vibrational-rotational mixing.