The seven deadly sins: When computing crystal nucleation rates, the devil is in the details
The seven deadly sins: When computing crystal nucleation rates, the devil is in the details
复制标题
DOI：
10.1063/5.0055248
复制
发表时间：
2021-07-28
影响因子：
4.4
通讯作者：
Sosso, Gabriele C.
中科院分区：
文献类型：
--
作者：
Blow, Katarina E.;Quigley, David;Sosso, Gabriele C.
晶体的形成已被证明是最具挑战性的相变定量模型之一，更不用说实际理解，无论是通过最新的实验技术或我们所掌握的增强采样方法的全部武器库。与结晶过程有关的最关键的量之一是成核速率，这是一个难以理解的数字，用来量化在一定体积和时间跨度内出现临界尺寸的核的平均概率。大量的努力已经致力于尝试通过原子模拟计算的晶体成核速率和它们的实验测量的对应物之间的连接。可悲的是，这一奋进几乎总是在某种程度上失败，而古老的经典成核理论通常被指责为罪魁祸首。在这里，我们回顾了该领域的一些最新进展，重点是一些可能更微妙的细节，有时被忽视时，计算成核率。我们认为，重要的是要让社区意识到各个方面的全面影响，例如有限尺寸效应和缓慢的动态，这些方面往往会在我们的模拟中引入不明显但不可忽视的不确定性来源。事实上，关键是要获得强大的和可重复的趋势，以便对过程的动力学，晶体成核的动力学，提供新的认识，这涉及到无数的实际应用，从药物的配制到纳米电子设备的制造。
The formation of crystals has proven to be one of the most challenging phase transformations to quantitatively model-let alone to actually understand-be it by means of the latest experimental technique or the full arsenal of enhanced sampling approaches at our disposal. One of the most crucial quantities involved with the crystallization process is the nucleation rate, a single elusive number that is supposed to quantify the average probability for a nucleus of critical size to occur within a certain volume and time span. A substantial amount of effort has been devoted to attempt a connection between the crystal nucleation rates computed by means of atomistic simulations and their experimentally measured counterparts. Sadly, this endeavor almost invariably fails to some extent, with the venerable classical nucleation theory typically blamed as the main culprit. Here, we review some of the recent advances in the field, focusing on a number of perhaps more subtle details that are sometimes overlooked when computing nucleation rates. We believe it is important for the community to be aware of the full impact of aspects, such as finite size effects and slow dynamics, that often introduce inconspicuous and yet non-negligible sources of uncertainty into our simulations. In fact, it is key to obtain robust and reproducible trends to be leveraged so as to shed new light on the kinetics of a process, that of crystal nucleation, which is involved into countless practical applications, from the formulation of pharmaceutical drugs to the manufacturing of nano-electronic devices.