Smessaert Anton, Rottler Jörg
Department of Physics and Astronomy, The University of British Columbia, 6224 Agricultural Road, Vancouver, British Columbia, Canada, V6T 1Z1.
Phys Rev E Stat Nonlin Soft Matter Phys. 2013 Aug;88(2):022314. doi: 10.1103/PhysRevE.88.022314. Epub 2013 Aug 26.
We investigate the spatiotemporal distribution of microscopic relaxation events, defined through particle hops, in a model polymer glass using molecular dynamics simulations. We introduce an efficient algorithm to directly identify hops during the simulation, which allows the creation of a map of relaxation events for the whole system. Based on this map, we present density-density correlations between hops and directly extract correlation scales. These scales define collaboratively rearranging groups of particles and their size distributions are presented as a function of temperature and age. Dynamical heterogeneity is spatially resolved as the aggregation of hops into clusters, and we analyze their volume distribution and growth during aging. A direct comparison with the four-point dynamical susceptibility χ(4) reveals the formation of a single dominating cluster prior to the χ(4) peak, which indicates maximally correlated dynamics. An analysis of the fractal dimension of the hop clusters finds slightly noncompact shapes in excellent agreement with independent estimates from four-point correlations.
我们使用分子动力学模拟研究了模型聚合物玻璃中通过粒子跳跃定义的微观弛豫事件的时空分布。我们引入了一种高效算法,以便在模拟过程中直接识别跳跃,这使得能够创建整个系统的弛豫事件图。基于此图,我们给出了跳跃之间的密度-密度相关性,并直接提取相关尺度。这些尺度定义了协同重排的粒子组,并且它们的尺寸分布作为温度和老化时间的函数给出。动态非均匀性在空间上表现为跳跃聚集成簇,我们分析了它们在老化过程中的体积分布和生长情况。与四点动态磁化率χ(4)的直接比较揭示了在χ(4)峰值之前形成了单个主导簇,这表明动力学具有最大相关性。对跳跃簇的分形维数的分析发现其形状略不紧凑,这与来自四点相关性的独立估计非常吻合。