Aggregation-volume-bias Monte Carlo simulations of vapor-liquid nucleation barriers for Lennard-Jonesium

Abstract

A combination of the aggregation-volume-bias Monte Carlo algorithm and the umbrella sampling technique is applied to investigate homogeneous vapor–liquid nucleation. This combined approach is simple, general, and robust. Its efficiency is demonstrated for nucleation of Lennard-Jonesium, for which the precise calculation of the nucleation barriers takes only a few minutes at higher supersaturations to a few hours at lower supersaturations. Comparison of the simulation results to the classical nucleation theory (CNT) shows that CNT overestimates the barrier heights by a value nearly independent of the supersaturation, but provides a reasonable description of the critical cluster sizes.