论文标题
经典成核理论：二阶校正热力学参数
Classical nucleation theory of ice nucleation: second-order correction of thermodynamic parameters
论文作者
论文摘要
成核速率的准确估计对于研究冰成核和促进冰冻/抗冻结策略至关重要。在经典成核理论（CNT）的框架内，冰成核速率的估计值对热力学参数非常敏感，例如水和冰$Δμ$和冰水室内室内自由能$γ$之间的化学势差。然而，即使在今天，估计这些热力学参数仍然存在许多矛盾和近似值，这对冰核率的估计值引入了巨大的不确定性。从基本概念开始，对于一般的固定液体结晶系统，我们将Gibbs-Thomson（GT）方程式扩展到二阶，并通过结合分子动力学（MD）模拟的二阶分析公式，$ ugig $ $ $δμ$，$γ$和核定屏障$ΔG$。这些公式很好地描述了这些热力学参数的温度依赖性。我们的结果可以提供估计$Δμ$，$γ$和$ΔG$的方法。
Accurate estimate of nucleation rate is crucial for the study of ice nucleation and ice-promoting/anti-freeze strategies. Within the framework of Classical Nucleation Theory (CNT), the estimate of ice nucleation rate is very sensitive to thermodynamic parameters, such as chemical potential difference between water and ice $Δμ$ and ice-water interfacial free energy $γ$. However, even today, there are still many contradictions and approximations in the estimating of these thermodynamic parameters, introducing large uncertainty to the estimate of the ice nucleation rate. Herein, starting from the basic concepts, for a general solid-liquid crystallization system, we expand the Gibbs-Thomson (GT) equation to second order, and derive the second-order analytical formulas of $Δμ$, $γ$ and nucleation barrier $ΔG$ with combining molecular dynamics (MD) simulations. These formulas describe well the temperature dependence of these thermodynamic parameters. Our results can provide a method of estimating $Δμ$, $γ$ and $ΔG$.
