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A new theoretical approach is presented for vapor-phase nucleation. In contrast to previous molecular approaches to nucleation that focus on evaluating equilibrium distributions of clusters, we evaluate rate constants for cluster evaporation and condensation that are the elementary kinetic steps in the nucleation mechanism. The use of variational transition state theory to estimate the rate constants provides a consistent procedure for defining a unique value for the constraining volume of the physically consistent cluster. The theory is applied to evaporation of small water clusters.
Schenter et al. (Mon,) studied this question.