Corezzi S, Fioretto D, Kenny J M
Dipartimento di Fisica, Università di Roma "La Sapienza", P. le A. Moro 2, I-00185 Roma, Italy.
Phys Rev Lett. 2005 Feb 18;94(6):065702. doi: 10.1103/PhysRevLett.94.065702.
We study the dependence of the dynamics on the size of particle clusters that grow by stepwise aggregation in a reactive epoxy-amine mixture. The data reveal the cluster property involved in the glasslike arrest and its quantitative link with the structural relaxation time. We find that the number-average cluster size xn governs the formation of a glassy phase as distinct from a gel phase, and that xn correlates to the size of the "cooperatively rearranging regions" postulated by the Adam-Gibbs model for glass forming liquids. These results suggest that the step polymerization process generates clusters that behave much like dynamical heterogeneities observed in supercooled liquids.
我们研究了动力学对反应性环氧 - 胺混合物中通过逐步聚集生长的粒子簇尺寸的依赖性。数据揭示了与玻璃态停滞相关的簇性质及其与结构弛豫时间的定量联系。我们发现,数均簇尺寸xn决定了玻璃相的形成,与凝胶相不同,并且xn与玻璃形成液体的Adam - Gibbs模型所假设的“协同重排区域”的尺寸相关。这些结果表明,逐步聚合过程产生的簇的行为与在过冷液体中观察到的动力学不均匀性非常相似。