Abstract
Vibrational relaxation of the OH stretching and bending modes of water monomers in acetonitrile is studied by two-color pump–probe experiments in a frequency range from 1400 to 3800cm−1. Measurements with resonant infrared excitation reveal vibrational lifetimes of 6.4±1.0ps of the OH stretching modes and 4.0±0.5ps of the OH bending mode. After OH stretching excitation, the OH bending mode shows an instantaneous response, a hallmark of the anharmonic coupling of stretching and bending modes, and a delayed population buildup by relaxation of the stretching via the bending mode. The relaxation steps are discussed within the framework of current theoretical pictures of water’s vibrational relaxation.
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