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In surveying the development of the field of gas-phase energy transfer, it is possible to identify three major phases of activity in the past 25 years. This is particularly the case for rotational energy transfer (RET), which is the main topic of this review, but to a lesser degree the same applies to other forms of energy transfer. As one might imagine, these phases of activity are closely associated with the development of experimental tech niques for the study of gas phase processes at more and more intimate levels. However, advances in the methods and techniques of performing theoretical calculations and improvements in computational power have also contributed to the current level of understanding of molecular collision dynamics.

The first of these phases corresponds to the early years, in which bulk relaxation measurements provided the main experimental data on energy transfer. Sound waves, shock waves, and …