Structural and conformational dynamics of supercooled polymer melts: Insights from first-principles theory and simulations
Structural and conformational dynamics of supercooled polymer melts: Insights from first-principles theory and simulations
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DOI：
10.1103/physreve.76.051806
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发表时间：
2007-11-01
影响因子：
2.4
通讯作者：
Baschnagel, Joerg
中科院分区：
文献类型：
--
作者：
Chong, Song-Ho;Aichele, Martin;Baschnagel, Joerg
对过冷、无纠缠的聚合物熔体的结构和构象动力学进行了微珠弹簧模型模拟和模耦合理论计算，并进行了定量比较。我们发现，除了在可压缩平台和静态结构因子的无定形晕之间的中等长度尺度上发生的过程外，模拟结果与理论结果是半定量一致的。我们的结果表明，玻璃形成熔体的缓慢松弛可以用单体笼化和链连接来描述。此外，从我们的理论中出现了(渐近地)遵循Rouse模型的玻璃化停滞和构象涨落的统一原子描述。
We report on quantitative comparisons between simulation results of a bead-spring model and mode-coupling theory calculations for the structural and conformational dynamics of a supercooled, unentangled polymer melt. We find semiquantitative agreement between simulation and theory, except for processes that occur on intermediate length scales between the compressibility plateau and the amorphous halo of the static structure factor. Our results suggest that the onset of slow relaxation in a glass-forming melt can be described in terms of monomer caging supplemented by chain connectivity. Furthermore, a unified atomistic description of glassy arrest and of conformational fluctuations that (asymptotically) follow the Rouse model emerges from our theory.