论文标题
分子模拟可以可靠地比较均质和异质冰核吗？
Can molecular simulations reliably compare homogeneous and heterogeneous ice nucleation?
论文作者
论文摘要
原则上，提出的名义问题的答案无疑是“是”。但是实际上，通过对通常用于异质系统使用的分子间相互作用的处理，获得了均质系统的必要参考数据。在本文中，我们评估了在比较均匀和不均匀环境中的水时选择截断方案的影响。具体而言，我们使用明确的自由能计算和简单的平均场分析来证明，使用Lennard-Jones潜力的“切换”版本（最简单的水的最简单点电荷模型）会导致冰I $ $ _ {\ rm H} $的系统升高。此外，通过对截止变化和压力变化之间的类比，我们使用现有的文献数据在负压下以均匀的冰成核来表明，由于多个幅度的数量级，由于异质成核引起的增强可能已经高估了。
In principle, the answer to the posed titular question is undoubtedly 'yes.' But in practice, requisite reference data for homogeneous systems have been obtained with a treatment of intermolecular interactions that is different from that typically employed for heterogeneous systems. In this article, we assess the impact of the choice of truncation scheme when comparing water in homogeneous and inhomogeneous environments. Specifically, we use explicit free energy calculations and a simple mean field analysis to demonstrate that using the 'cut-and-shift' version of the Lennard-Jones potential (common to most simple point charge models of water) results in a systematic increase in the melting temperature of ice I$_{\rm h}$. In addition, by drawing an analogy between a change in cutoff and a change in pressure, we use existing literature data for homogeneous ice nucleation at negative pressures to suggest that enhancements due to heterogeneous nucleation may have been overestimated by several orders of magnitude.
