Abstract
CH-stretching modes were first excited by picosecond infrared pulses and the generated excess population was monitored by anti-Stokes scattering of subsequent ultrashort probe pulses. Experimental data are reported on five molecules: CHCl 3, CH 2Cl 2, CH 3CCl 3, CH 3CH 2OH, and CH 3I in the neat liquid and/or in solutions of CCl 4. The observed time constants vary between 1 and 100 ps depending upon the individual molecule and surrounding. Theoretical calculations show that rotational coupling, Fermi resonance, Coriolis coupling, and resonance energy transfer can strongly effect the vibrational population lifetime. The relevance of these processes is quite different for the various molecules investigated.
Published Version
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