Equilibrium fluid-crystal interfacial free energy of bcc-crystallizing aqueous suspensions of polydisperse charged spheres.

Equilibrium fluid-crystal interfacial free energy of bcc-crystallizing aqueous suspensions of polydisperse charged spheres.
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多分散带电球体 bcc 结晶水悬浮液的平衡流体晶体界面自由能

DOI:
10.1103/physreve.93.022601
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发表时间:
2016
期刊:
Physical review. E
影响因子:
--
通讯作者:
D. M. Herlach
D. M. Herlach
中科院分区:
--
文献类型:
--
作者:
T. Palberg;P. Wette;D. M. Herlach

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界面自由能是亚稳熔体结晶过程中的一个中心量。在带电胶体球的悬浮液中,成核和生长动力学可以从光学实验中准确地测量。在以前的工作中,从这些数据有效的非平衡值之间的界面自由能新兴的体心立方核和相邻的熔体依赖于熔体相和结晶相之间的化学势差,使用经典的成核理论(CNT)。观察到界面自由能的严格线性增加作为增加的亚稳性的函数。在这里,我们进一步分析这些数据的五个带电球体和一个二元混合物的水悬浮液。我们利用一个简单的外推方案,并解释我们的研究结果,鉴于特恩布尔的经验规则。这使我们能够提出第一个系统的实验估计减少的界面自由能,bcc晶体相和共存的平衡流体之间。获得的值是在几个订单。它们的值是不相关的任何静电相互作用参数,而是显示出系统的减少,增加尺寸多分散性和较低的值的混合物相比,纯组分。同时,也与冻结熵呈近似线性相关。因此,严格单分散带电球体的平衡界面自由能可能更大。
The interfacial free energy is a central quantity in crystallization from the metastable melt. In suspensions of charged colloidal spheres, nucleation and growth kinetics can be accurately measured from optical experiments. In previous work, from these data effective nonequilibrium values for the interfacial free energy between the emerging bcc nuclei and the adjacent melt in dependence on the chemical potential difference between melt phase and crystal phase were derived using classical nucleation theory (CNT). A strictly linear increase of the interfacial free energy was observed as a function of increased metastability. Here, we further analyze these data for five aqueous suspensions of charged spheres and one binary mixture. We utilize a simple extrapolation scheme and interpret our findings in view of Turnbull's empirical rule. This enables us to present the first systematic experimental estimates for a reduced interfacial free energy,, between the bcc-crystal phase and the coexisting equilibrium fluid. Values obtained forare on the order of a few. Their values are not correlated to any of the electrostatic interaction parameters but rather show a systematic decrease with increasing size polydispersity and a lower value for the mixture as compared to the pure components. At the same time,also shows an approximately linear correlation to the entropy of freezing. The equilibrium interfacial free energy of strictly monodisperse charged spheres may therefore be still greater.
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