Abstract
A new formulation of the theory of vibrational relaxation, based on Zener's semiclassical approximation, is presented here. The relaxation rate is shown to be proportional to the spectral density of the force exerted on the oscillator by its environment. The isolated binary collision theory is derived, but only with the condition that the collision frequency is much smaller than the oscillator frequency. This requirement is not satisfied in a liquid; we conclude that Litovitz's application of the isolated binary collision theory to liquids is not justified. A possible relation between vibrational relaxation and the self-diffusion coefficient in a liquid is discussed.
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