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RESEARCH PRODUCT
Crystallization of hard spheres revisited. II. Thermodynamic modeling, nucleation work, and the surface of tension
David RichardThomas Specksubject
Work (thermodynamics)SpinodalMaterials scienceStatistical Mechanics (cond-mat.stat-mech)010304 chemical physicsNucleationFOS: Physical sciencesGeneral Physics and AstronomyThermodynamicsFluxHard spheresCondensed Matter - Soft Condensed MatterOrders of magnitude (numbers)01 natural scienceslaw.inventionPhysics::Fluid DynamicsSurface tensionlaw0103 physical sciencesSoft Condensed Matter (cond-mat.soft)Physical and Theoretical ChemistryCrystallization010306 general physicsCondensed Matter - Statistical Mechanicsdescription
Combining three numerical methods (forward flux sampling, seeding of droplets, and finite-size droplets), we probe the crystallization of hard spheres over the full range from close to coexistence to the spinodal regime. We show that all three methods allow us to sample different regimes and agree perfectly in the ranges where they overlap. By combining the nucleation work calculated from forward flux sampling of small droplets and the nucleation theorem, we show how to compute the nucleation work spanning three orders of magnitude. Using a variation of the nucleation theorem, we show how to extract the pressure difference between the solid droplet and ambient liquid. Moreover, combining the nucleation work with the pressure difference allows us to calculate the interfacial tension of small droplets. Our results demonstrate that employing bulk quantities yields inaccurate results for the nucleation rate.
| year | journal | country | edition | language |
|---|---|---|---|---|
| 2018-05-15 | The Journal of Chemical Physics |