Abstract
In recent years, experimental investigations of vibrational relaxation processes have received increasing attention. Interesting information is obtained from the band shapes observed in infrared and Raman spectroscopy [1, 21. The interpretation of the measured lines is difficult, however, since several physical processes contribute in general to the observed band contours. Line broadening factors are: rotational motion, vibrational dephasing, energy relaxation, and inhomogeneous broadening due to a distribution of vibrational frequencies, e.g. isotopic line splitting. Under certain assumptions it is possible to separate the rotational contribution. The rest is sometimes called the “intrinsic vibrational part” and contains the other line-broadening factors. At the present time, one cannot isolate the different contributions by spectroscopic methods. For instance, the population lifetime of an excited vibrational state was unknown until very recently for any vibrational mode in the liquid state. Similarly, the inhomogeneous part of a spectroscopic line is not known in many cases. As a result, the time constants deduced from spectroscopic band contours are not well understood.
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Laubereau, A., Kaiser, W. (1978). Picosecond Laser Techniques. In: Dupuy, J., Dianoux, A.J. (eds) Microscopic Structure and Dynamics of Liquids. NATO Advanced Study Institutes Series, vol 33. Springer, Boston, MA. https://doi.org/10.1007/978-1-4684-0859-1_8
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