Iacopini Sara, Palberg Thomas, Schöpe Hans Joachim
Institut fur Physik, Johannes Gutenberg Universitat Mainz, Staudingerweg 7, D-55128 Mainz, Germany.
J Chem Phys. 2009 Feb 28;130(8):084502. doi: 10.1063/1.3078310.
Highly cross-linked polystyrene microgel colloids dispersed in an index and density matching solvent provide a system with hard-sphere-like interactions, where gravity effects are effectively minimized. They are a suitable target for time-resolved observations of solidification in purely repulsive systems. We have investigated the crystallization kinetics at increasing undercooling using time resolved light scattering. Crystallization starts always with the formation of compressed, structurally heterogeneous precursor domains. In the coexistence region the precursors, after being converted into true crystallites, start growing fast by assimilating particles from the melt. The resulting polycrystalline material consists of high quality crystals and seems not to undergo long time-scale rearrangements. As the particle concentration grows, the higher undercooling and reduced particle mobility increasingly compromise the conversion-growth process. The growth of crystallites relies then on much slower ripeninglike processes, while refining of the crystal structure is detected up to the longest observed times.
分散在折射率和密度匹配溶剂中的高度交联聚苯乙烯微凝胶胶体提供了一个具有类似硬球相互作用的系统,其中重力效应被有效最小化。它们是在纯排斥系统中对凝固进行时间分辨观测的合适目标。我们使用时间分辨光散射研究了过冷度增加时的结晶动力学。结晶总是从形成压缩的、结构不均匀的前驱体域开始。在共存区域,前驱体在转化为真正的微晶后,通过从熔体中吸收粒子开始快速生长。所得的多晶材料由高质量的晶体组成,似乎不会经历长时间尺度的重排。随着颗粒浓度的增加,更高的过冷度和降低的颗粒迁移率越来越不利于转化-生长过程。微晶的生长随后依赖于慢得多的类熟化过程,而在最长的观测时间内都能检测到晶体结构的细化。