6533b85dfe1ef96bd12be047
RESEARCH PRODUCT
Crystallization of hard spheres revisited. I. Extracting kinetics and free energy landscape from forward flux sampling
Thomas SpeckDavid Richardsubject
PhysicsStatistical Mechanics (cond-mat.stat-mech)NucleationGeneral Physics and AstronomyEnergy landscapeSampling (statistics)FOS: Physical sciencesHard spheresCondensed Matter - Soft Condensed Matter010402 general chemistry01 natural sciences0104 chemical sciencesSurface tensionMetastability0103 physical sciencesSoft Condensed Matter (cond-mat.soft)Statistical physicsClassical nucleation theoryPhysical and Theoretical Chemistry010306 general physicsScalingCondensed Matter - Statistical Mechanicsdescription
We investigate the kinetics and the free energy landscape of the crystallization of hard spheres from a supersaturated metastable liquid though direct simulations and forward flux sampling. In this first paper, we describe and test two different ways to reconstruct the free energy barriers from the sampled steady state probability distribution of cluster sizes without sampling the equilibrium distribution. The first method is based on mean first passage times, and the second method is based on splitting probabilities. We verify both methods for a single particle moving in a double-well potential. For the nucleation of hard spheres, these methods allow us to probe a wide range of supersaturations and to reconstruct the kinetics and the free energy landscape from the same simulation. Results are consistent with the scaling predicted by classical nucleation theory although a quantitative fit requires a rather large effective interfacial tension.
| year | journal | country | edition | language |
|---|---|---|---|---|
| 2018-03-28 |