Mean-square fluctuations about a correlation function in its approach to equilibrium are defined and studied. For the case of a correlation function for molecular reorientation, it is shown that this time-dependent fluctuation can be evaluated by combining experimental infrared and Raman band shapes. Examples are given for liquid CO and CH4. The experiments suggest that nonequilibrium fluctuations approach their equilibrium values faster than do the corresponding average correlations.
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Roy G. Gordon (1967) studied this question.
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