Finite size effects on liquid-solid phase coexistence and the estimation of crystal nucleation barriers

الأصل · EN

A fluid in equilibrium in a finite volume V with particle number N at a density ρ= N/V exceeding the onset density ρf of freezing may exhibit phase coexistence between a crystalline nucleus and surrounding fluid. Using a method suitable for the estimation of the chemical potential of dense fluids we obtain the excess free energy due to the surface of the crystalline nucleus. There is neither a need to precisely locate the interface nor to compute the (anisotropic) interfacial tension. As a test case, a soft version of the Asakura-Oosawa model for colloid polymer-mixtures is treated. While our analysis is appropriate for crystal nuclei of arbitrary shape, we find the nucleation barrier to be compatible with a spherical shape, and consistent with classical nucleation theory.