Molecular Dynamics Based Analysis of Nucleation and Surface Energy of Droplets in Supersaturated Vapors of Methane and Ethane

Homogeneous nucleation processes are characterized by the nucleation rate and the critical droplet size. Molecular dynamics (MD) simulation is applied for studying homogeneous nucleation during condensation of supersaturated vapors of methane and ethane. The results are compared to the classical nucleation theory (CNT) and the Laaksonen-Ford-Kulmala (LFK) model that introduces a size dependence of the specific surface energy. It is shown for the nucleation rate that the Yasuoka-Matsumoto method and the mean first passage time (MFPT) method lead to considerably differing results. Even more significant deviations are found between two other approaches to the critical droplet size, based on the maximum of the Gibbs free energy of droplet formation (Yasuoka-Matsumoto) and the supersaturation dependence of the nucleation rate (nucleation theorem). CNT is found to agree reasonably well with the simulation results, whereas LFK leads to large deviations at high temperatures