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From compact to fractal crystalline clusters in concentrated systems of monodisperse hard spheres

机译:从浓缩系统中的致密晶体团簇到分形晶体团簇   单分散硬球

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摘要

We address the crystallization of monodisperse hard spheres in terms of theproperties of finite- size crystalline clusters. By means of large scaleevent-driven Molecular Dynamics simulations, we study systems at differentpacking fractions {\phi} ranging from weakly supersaturated state points toglassy ones, covering different nucleation regimes. We find that such regimesalso result in different properties of the crystalline clusters: compactclusters are formed in the classical-nucleation-theory regime ({\phi} \leq0.54), while a crossover to fractal, ramified clusters is encountered uponincreasing packing fraction ({\phi} \geq 0.56), where nucleation is morespinodal-like. We draw an analogy between macroscopic crystallization of ourclusters and percolation of attractive systems to provide ideas on how thepacking fraction influences the final structure of the macroscopic crystals. Inour previous work (Phys. Rev. Lett., 106, 215701, 2011), we have demonstratedhow crystallization from a glass (at {\phi} > 0.58) happens via a gradual(many-step) mechanism: in this paper we show how the mechanism of gradualgrowth seems to hold also in super-saturated systems just above freezingshowing that static properties of clusters are not much affected by dynamics.
机译:根据有限尺寸的晶体簇的性质,我们解决了单分散硬球的结晶问题。通过大规模事件驱动的分子动力学模拟,我们研究了从弱过饱和状态点到玻璃态的不同堆积分数{\ phi}的系统,涵盖了不同的成核机制。我们发现,这样的晶格也会导致晶体团簇的不同性质:在经典成核理论体系({\ phi} \ leq0.54)中形成紧密团簇,而随着堆积分数的增加,会遇到分形,分枝的团簇的穿越( {\ phi} \ geq 0.56),其中形核类似于螺齿状。我们在簇的宏观结晶与有吸引力的系统的渗滤之间进行类比,以提供有关堆积分数如何影响宏观晶体最终结构的想法。在我们以前的工作(Phys。Rev. Lett。,106,215701,2011)中,我们已经证明了玻璃的结晶(在{\ phi}> 0.58时)是如何通过渐进(多步)机制发生的:在本文中,我们展示了渐增机制在冰点以上的超饱和系统中似乎如何保持不变,这表明簇的静态属性受动力学影响不大。

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