2010/06/15 by L. Filion, Laura Filion, M. Hermes +5 · 2 citations
Earth and Planetary Sciences · Engineering · Materials Science · Physics and Astronomy · #Classical nucleation theory #Crystal (programming language) #Diffusion #Flux (metallurgy) #Hard spheres #Material Dynamics and Properties #Molecular dynamics #Nucleation #Phase Equilibria and Thermodynamics #SPHERES #cond-mat.soft #nanoparticles nucleation surface interactions
paper · pdf · doi:10.1063/1.3506838
published as J. Chem. Phys., 2010, 133, 244115 · Submitted to the Journal of Chemical Physics
arxiv created 2010/06/15 · openalex publication_date 2010/12/28 · arxiv updated 2012/08/17 · openalex created_date 2016/06/24 · openalex updated_date 2026/08/05
Over the last number of years several simulation methods have been introduced to study rare events such as nucleation. In this paper we examine the crystal nucleation rate of hard spheres using three such numerical techniques: molecular dynamics, forward flux sampling, and a Bennett-Chandler-type theory where the nucleation barrier is determined using umbrella sampling simulations. The resulting nucleation rates are compared with the experimental rates of Harland and van Megen [Phys. Rev. E 55, 3054 (1997)], Sinn et al. [Prog. Colloid Polym. Sci. 118, 266 (2001)], Schätzel and Ackerson [Phys. Rev. E 48, 3766 (1993)], and the predicted rates for monodisperse and 5% polydisperse hard spheres of Auer and Frenkel [Nature 409, 1020 (2001)]. When the rates are examined in units of the long-time diffusion coefficient, we find agreement between all the theoretically predicted nucleation rates, however, the experimental results display a markedly different behavior for low supersaturation. Additionally, we examined the precritical nuclei arising in the molecular dynamics, forward flux sampling, and umbrella sampling simulations. The structure of the nuclei appears independent of the simulation method, and in all cases, the nuclei contains on average significantly more face-centered-cubic ordered particles than hexagonal-close-packed ordered particles.