液体中的晶体成核：分子动力学模拟中的悬而未决的问题和未来的挑战,Chemical Reviews

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液体中的晶体成核：分子动力学模拟中的悬而未决的问题和未来的挑战
Chemical Reviews ( IF 51.4 ) Pub Date : 2016-05-26 00:00:00 , DOI: 10.1021/acs.chemrev.5b00744
Gabriele C Sosso ₁ , Ji Chen ₁ , Stephen J Cox ₁ , Martin Fitzner ₁ , Philipp Pedevilla ₁ , Andrea Zen ₁ , Angelos Michaelides ₁

Affiliation

液体中晶体的成核是自然界最普遍的现象之一，在气候变化和药物生产等领域发挥着重要作用。由于成核的早期阶段涉及极小的时间和长度尺度，原子计算机模拟可以提供对结晶微观方面的独特见解。在这篇综述中，我们盘点了过去几十年中众多的分子动力学模拟，这些模拟揭示了液体中晶体成核的关键方面。我们通过回顾冰成核和溶液中分子结晶等过程的模拟，将经典成核理论的理论框架和最先进的计算方法置于背景中。我们将看到，分子动力学模拟为从胶体颗粒到天然气水合物的各种成核场景提供了关键见解，因此，经典成核理论的普遍适用性一再受到质疑。我们试图找出该领域最紧迫的开放性问题。我们相信，通过改进（i）现有的原子间势和（ii）当前可用的增强采样方法，社区可以朝着对实际感兴趣的现实系统进行准确研究的方向发展，从而使模拟更接近实验。

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Crystal Nucleation in Liquids: Open Questions and Future Challenges in Molecular Dynamics Simulations

The nucleation of crystals in liquids is one of nature’s most ubiquitous phenomena, playing an important role in areas such as climate change and the production of drugs. As the early stages of nucleation involve exceedingly small time and length scales, atomistic computer simulations can provide unique insights into the microscopic aspects of crystallization. In this review, we take stock of the numerous molecular dynamics simulations that, in the past few decades, have unraveled crucial aspects of crystal nucleation in liquids. We put into context the theoretical framework of classical nucleation theory and the state-of-the-art computational methods by reviewing simulations of such processes as ice nucleation and the crystallization of molecules in solutions. We shall see that molecular dynamics simulations have provided key insights into diverse nucleation scenarios, ranging from colloidal particles to natural gas hydrates, and that, as a result, the general applicability of classical nucleation theory has been repeatedly called into question. We have attempted to identify the most pressing open questions in the field. We believe that, by improving (i) existing interatomic potentials and (ii) currently available enhanced sampling methods, the community can move toward accurate investigations of realistic systems of practical interest, thus bringing simulations a step closer to experiments.

更新日期：2016-05-26

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