Institut für Physik, Johannes Gutenberg-Universität Mainz, Staudinger Weg 9, 55128 Mainz, Germany and Graduate School of Excellence Materials Science in Mainz, Staudinger Weg 9, 55128 Mainz, Germany.
Institut für Physik, Johannes Gutenberg-Universität Mainz, Staudinger Weg 9, 55128 Mainz, Germany.
Phys Rev Lett. 2015 Jan 16;114(2):026101. doi: 10.1103/PhysRevLett.114.026101. Epub 2015 Jan 13.
A fluid in equilibrium in a finite volume V with particle number N at a density ρ=N/V exceeding the onset density ρ_{f} 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.
在有限体积 V 中处于平衡状态的流体，其粒子数 N 达到起始冻结密度 ρ_{f}以上时，即 ρ=N/V，可能会在结晶核与周围流体之间表现出相共存。我们使用一种适用于估算稠密流体化学势的方法，得到了由于结晶核表面而产生的过剩自由能。既不需要精确地定位界面，也不需要计算（各向异性的）界面张力。作为一个测试案例，我们处理了胶体-聚合物混合物的 Asakura-Oosawa 模型的软版本。虽然我们的分析适用于任意形状的晶体核，但我们发现成核势垒与球形相容，并且与经典成核理论一致。
