In this work, we use molecular dynamics simulations with a polarizable force field, namely, the modified AH/BK3 model [J. Kolafa, J. Chem. Phys. 145, 204509 (2016)], in combination with the forward flux sampling technique, to calculate the rates of homogeneous nucleation of NaCl from supersaturated aqueous solutions at 298 K and 1 bar. A non-polarizable model that reproduces the experimental equilibrium solubility {AH/TIP4P-2005 of Benavides et al. [J. Chem. Phys. 147, 104501 (2017)]} is also used for comparison. Nucleation rates calculated from the polarizable force field are found to be in good agreement with experimental measurements, while the non-polarizable model severely underestimates the nucleation rates. These results, in combination with our earlier study of a different non-polarizable force field [H. Jiang et al., J. Chem. Phys. 148, 044505 (2018)], lead to the conclusion that nucleation rates are sensitive to the details of force fields, and a good representation of nucleation rates may not be feasible using available non-polarizable force fields, even if these reproduce the equilibrium salt solubility. Inclusion of polarization could be important for an accurate prediction of nucleation rates in salt solutions.

中文翻译：

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通讯：使用极化力场的过饱和NaCl水溶液的成核速率

在这项工作中，我们使用具有可极化力场的分子动力学模拟，即改进的AH / BK3模型[J. Kolafa，J.Chem。物理 145，204509（2016）]，在与前向磁通采样技术组合，以从在298K和1巴的过饱和水溶液的NaCl计算的均相成核的发生率。一种不可极化的模型，可重现Benavides等人的实验平衡溶解度{AH / TIP4P-2005 。[J. 化学 物理 147，104501（2017）]}也用于比较。发现由可极化力场计算出的成核率与实验测量值非常吻合，而不可极化模型则严重低估了成核率。这些结果，结合我们先前对不同的不可极化力场的研究[H. 江等。，J. Chem。物理 148，044505（2018）]，铅的结论是，成核速率是力场的细节敏感，并且使用可用的不可极化的力场成核速率的良好表示可能是不可行的，即使这些重现平衡盐溶解度。包含极化对于准确预测盐溶液中的成核速率可能很重要。