We employ density functional theory to explore the range of validity of phenomenological approaches to the study of gas-liquid nucleation. We consider the Dillmann-Meier theory of nucleation and the diffuse interface theory developed by Gránásy. By using density functional theory to calculate cluster properties such as the variation of free energy with cluster size or the local enthalpy or entropy profiles, we find that the success of these models in fitting experimental data is at least in part fortuitous. On the basis of our analysis, we identify relevant model variables and propose new parametrizations that are more consistent with our density functional calculations.
ASJC Scopus subject areas
- General Engineering
- Physical and Theoretical Chemistry