MONTE-CARLO RECURSION STUDY OF CLUSTER FORMATION FROM VAPOR

A general formalism of cluster formation from monatomic vapor is developed, based on classical statistical mechanics in the isothermal-isobaric ensemble. The Gibbs free energy of clusters in a constrained equilibrium with vapor can be computed efficiently using a Monte Carlo recursion procedure. The application of our theory and method to the study of homogeneous nucleation of argon clusters shows that small clusters under supersaturation conditions tend to have lower effective density compared with the corresponding bulk liquid, and more negative Gibbs free energy of formation than that predicted from the classical nucleation theory. © 1990 American Institute of Physics.