论文标题
单个冷凝聚合物中玻璃动力学的RFOT理论
RFOT theory for glassy dynamics in a single condensed polymer
论文作者
论文摘要
单个冷凝聚合物(SCP)的紧凑结构的数量,具有相似的自由能,随着聚合的程度呈指数增长。与结构玻璃(SG)类似,我们预计在低温下,应通过紧凑型亚稳态状态之间的过渡发生链条弛豫。通过将线性耦合到参考状态的SCP的状态发展,我们表明,在动态过渡温度($ t_d $)下方,SCP被困在亚稳态状态下,导致动力学缓慢。在较低的温度下,$ t_k \ ne 0 $,配置熵消失,导致热力学随机一阶理想玻璃过渡。放松时间遵守Vogel-Fulcher-Tamman定律,以$ t = t_0 \ of t_k $分歧。这些发现符合随机的一级过渡理论,确定SCP和SG表现出相似的普遍特征。
The number of compact structures of a single condensed polymer (SCP), with similar free energies, grows exponentially with the degree of polymerization. In analogy with structural glasses (SGs), we expect that at low temperatures chain relaxation should occur by activated transitions between the compact metastable states. By evolving the states of the SCP that is linearly coupled to a reference state, we show that, below a dynamical transition temperature ($T_d$), the SCP is trapped in a metastable state leading to slow dynamics. At a lower temperature, $T_K \ne 0$, the configurational entropy vanishes, resulting in a thermodynamic random first order ideal glass transition. The relaxation time obeys the Vogel-Fulcher-Tamman law, diverging at $T=T_0 \approx T_K$. These findings, accord well with the random first order transition theory, establishing that SCP and SG exhibit similar universal characteristics.