硬棒成核的玻璃态动力学、旋节涨落和动力学极限
Glassy dynamics, spinodal fluctuations, and the kinetic limit of hard-rod nucleation
摘要:
利用模拟,我们确定了三个动力学制度在过饱和各向同性流体状态的短硬棒:(i)对于中度过饱和,我们观察到成核的多层晶体团簇;(ii)在较高的过饱和度下,我们发现小晶粒的成核,其排列成长寿命的局部有利结构,其在动力学上被阻止,而(iii)在甚至更高的过饱和度下,动态停滞是由于常规的笼捕集玻璃化转变。对于较长的杆,我们发现,形成的(稳定)近晶相的过饱和各向同性的状态强烈抑制各向同性的spinodal不稳定性,导致巨大的spinodal样的取向波动与spinodal集群分散的大小。我们的研究结果表明,玻璃态动力学和调幅不稳定性设置动力学限制成核在一个高度过饱和的硬棒流体。
英文摘要:
Using simulations we identify three dynamic regimes in supersaturated isotropic fluid states of short hard rods: (i) for moderate supersaturations we observe nucleation of multi-layered crystalline clusters; (ii) at higher supersaturation, we find nucleation of small crystallites which arrange into long-lived locally favored structures that get kinetically arrested, while (iii) at even higher supersaturation the dynamic arrest is due to the conventional cage-trapping glass transition. For longer rods we find that the formation of the (stable) smectic phase out of a supersaturated isotropic state is strongly suppressed by an isotropic-nematic spinodal instability that causes huge spinodal-like orientation fluctuations with nematic clusters diverging in size. Our results show that glassy dynamics and spinodal instabilities set kinetic limits to nucleation in a highly supersaturated hard-rod fluids.
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