3 research outputs found
Crystallization in suspensions of hard spheres: A Monte Carlo and Molecular Dynamics simulation study
The crystallization of a metastable melt is one of the most important non
equilibrium phenomena in condensed matter physics, and hard sphere colloidal
model systems have been used for several decades to investigate this process by
experimental observation and computer simulation. Nevertheless, there is still
an unexplained discrepancy between simulation data and experimental nucleation
rate densities. In this paper we examine the nucleation process in hard spheres
using molecular dynamics and Monte Carlo simulation. We show that the
crystallization process is mediated by precursors of low orientational
bond-order and that our simulation data fairly match the experimental data
sets
Crystal nucleation of hard spheres using molecular dynamics, umbrella sampling, and forward flux sampling: a comparison of simulation techniques
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–Chandlertype 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