A Molecular Theory of the Homogeneous Nucleation of Ice from Supercooled Water.

摘要

The investigation is an attempt to obtain reliable theoretical values for the surface free energies of ice embryos in supercooled water and thereby to obtain a fully determined theoretical description of the homogeneous nucleation of ice which may be meaningfully compared with experimental data. A statistical thermodynamic model of liquid water is developed and used to extract,from thermodynamic data on liquid water,information relevant to the molecular interactions at an ice-water interface. This model is used as the basis for a statistical thermodynamic evaluation of the surface and edge contributions to the free energy of formation of an ice embryo from supercooled water. The theoretical results for the free energy of formation of an ice embryo are incorporated into framework of quasi-thermodynamic nucleation theory and curves for the mean freezing temperature of pure water droplets as a function of droplet diameter are calculated for several cooling rates. (Author)