The unique role of bond length in the glassy dynamics of colloidal polymers

The unique role of bond length in the glassy dynamics of colloidal polymers
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键长在胶体聚合物玻璃态动力学中的独特作用

DOI:
10.1039/c6sm01386d
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发表时间:
2016
期刊:
影响因子:
3.4
通讯作者:
Ma Yu-qiang
Ma Yu-qiang
中科院分区:
化学2区
文献类型:
--
作者:
Zhang Bo-kai;Li Hui-shu;Li Jian;Chen Kang;Tian Wen-de;Ma Yu-qiang

文献摘要

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键长通常不被认为是分子聚合物的可控变量。因此,没有实验,模拟或理论研究,据我们所知,研究了键长对聚合物的玻璃态动力学的影响。近年来,人们合成了一类新型的组装材料,称为“胶体聚合物”。这些胶体聚合物在调节的可见性和灵活性方面优于分子聚合物,例如,“单体”的大小和形状、相互作用和键长。胶体聚合物的稠密悬浮体系将成为探索链状“分子”玻璃化转变基本问题的一个非常有前途的理想模型体系。本文将胶体非线性朗之万方程理论推广到胶体聚合物,研究了硬球胶体聚合物的静态结构和活化动力学。令人惊讶的是,我们发现键长在许多方面起着关键和独特的作用。例如,发现特征局部长度和活化势垒与“过冷度”以及结构弛豫与局部振动运动的普遍关系依赖于键长而与链长和刚性无关。我们希望我们的研究结果能启发未来的实验和模拟研究胶体聚合物的玻璃态动力学的研究。
Bond length is generally not considered as a controllable variable for molecular polymers. Hence, no experimental, simulation or theoretical research, to our knowledge, has examined the influence of bond length on the glassy dynamics of polymers. Recently, a new class of assembling materials called “colloidal polymers” has been synthesized. These colloidal polymers have advantages over molecular polymers in the visibility and flexibility of tuning, for example, the size and shape of the “monomers”, the interaction, and the bond length. Dense suspension of colloidal polymers will become a very promising ideal model system for exploring the fundamental problems in the glass transition of chain “molecules”. Here, we study the static structure and activated dynamics of hard-sphere colloidal polymers by generalizing the colloidal nonlinear Langevin equation theory to colloidal polymers. Surprisingly, we find that the bond length plays a critical and unique role in many aspects. For instance, the universal relations of the characteristic local lengths and the activated barrier versus the “degree of supercooling”, and the structural relaxation versus local vibrational motion are found to be dependent on bond length and independent of chain length and rigidity. We hope that our findings inspire future experimental and simulation research studies on the glassy dynamics of colloidal polymers.