2012/08/12 by James F. Lutsko
Earth and Planetary Sciences · Materials Science · Physics and Astronomy · #Advanced Thermodynamics and Statistical Mechanics #Material Dynamics and Properties #cond-mat.soft #cond-mat.stat-mech #nanoparticles nucleation surface interactions #physics.chem-ph
paper · pdf · doi:10.1063/1.4758454
published as J. Chem. Phys. 137, 154903 (2012)
arxiv created 2012/08/12 · openalex publication_date 2012/10/17 · arxiv updated 2012/10/18 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
A recently formulated description of homogeneous nucleation for Brownian particles in the over-damped limit based on fluctuating hydrodynamics is used to determine the nucleation pathway, characterized as the most likely path (MLP), for the nucleation of a dense-concentration droplet of globular protein from a dilute solution in a small, finite container. The calculations are performed by directly discretizing the equations for the MLP and it is found that they confirm previous results obtained for infinite systems: the process of homogeneous nucleation begins with a long-wavelength, spatially-extended concentration fluctuation that condenses to form the pre-critical cluster. This is followed by a classical growth processes. The calculations show that the post-critical growth involves the formation of a depletion zone around the cluster whereas no such depletion is observed in the pre-critical cluster. The approach therefore captures dynamical effects not found in classical density functional theory studies while consistently describing the formation of the pre-critical cluster.