Department of Physics, Wesleyan University, Middletown, Connecticut 06459, USA.
Phys Rev Lett. 2011 Mar 18;106(11):115702. doi: 10.1103/PhysRevLett.106.115702. Epub 2011 Mar 15.
We investigate the impact of nanoparticles (NP) on the fragility and cooperative stringlike motion in a model glass-forming polymer melt by molecular dynamics simulation. The NP cause significant changes to both the fragility and the average length of stringlike motion, where the effect depends on the NP-polymer interaction and NP concentration. We interpret these changes via the Adam-Gibbs (AG) theory, assuming the strings can be directly identified with the abstract "cooperatively rearranging regions" of AG. Our findings indicate that fragility is primarily a measure of the temperature dependence of the cooperativity of molecular motion.
我们通过分子动力学模拟研究了纳米粒子(NP)对模型玻璃形成聚合物熔体的脆性和协同串状运动的影响。NP 对脆性和串状运动的平均长度都有显著的影响,其影响取决于 NP-聚合物的相互作用和 NP 的浓度。我们通过 Adam-Gibbs(AG)理论来解释这些变化,假设这些串可以直接与 AG 的抽象“协同重排区域”相对应。我们的发现表明,脆性主要是分子运动协同性对温度依赖性的度量。