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Cluster Glasses of Semi?exible Ring Polymers

机译:半柔性环状聚合物簇玻璃

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摘要

We present computer simulations of concen- trated solutions of unknotted nonconcatenated semi?exible ring polymers. Unlike in their ?exible counterparts, shrinking involves a strong energetic penalty, favoring interpenetration and clustering of the rings. We investigate the slow dynamics of the centers-of-mass of the rings in the amorphous cluster phase, consisting of disordered columns of oblate rings penetrated by bundles of prolate ones. Scattering functions reveal a striking decoupling of self- and collective motions. Correlations between centers-of-mass exhibit slow relaxation, as expected for an incipient glass transition, indicating the dynamic arrest of the cluster positions. However, self-correlations decay at much shorter time scales. This feature is a manifestation of the fast, continuous exchange and diffusion of the individual rings over the matrix of clusters. Our results reveal a novel scenario of glass formation in a simple monodisperse system, characterized by self-collective decoupling, soft caging, and mild dynamic heterogeneity.
机译:我们介绍了未连接的非连接半柔性环聚合物的浓缩溶液的计算机模拟。与它们的弹性对应物不同,收缩涉及强大的能量损失,有利于环的互穿和聚集。我们研究了无定形簇相中环的质心的缓慢动力学,该环由扁圆环束穿透的扁圆环的无序列组成。散射函数揭示了自我运动和集体运动的惊人解耦。质量中心之间的相关性显示出缓慢的松弛,这是初期玻璃化转变所预期的,表明簇位置的动态停滞。但是,自相关在更短的时间尺度上衰减。该特征是各个环在簇矩阵上快速,连续交换和扩散的体现。我们的研究结果揭示了在简单的单分散体系中形成玻璃的新情况,其特征是具有自收集解耦,软笼养和温和的动态异质性。

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