Citation: Deng Pan, Zhao-Yan Sun. Diffusion and Relaxation Dynamics of Supercooled Polymer Melts[J]. Chinese Journal of Polymer Science, ;2018, 36(10): 1187-1194. doi: 10.1007/s10118-018-2132-9 shu

Diffusion and Relaxation Dynamics of Supercooled Polymer Melts

Deng Pan ^1,2 ,
Zhao-Yan Sun ^1,3,,

a.
State Key Laboratory of Polymer Physics and Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
b.
University of Chinese Academy of Sciences, Beijing 100049, China
c.
Xinjiang Laboratory of Phase Transitions and Microstructures in Condensed Matters, College of Physical Science and Technology, Yili Normal University, Yining 835000, China

Corresponding author: Zhao-Yan Sun, zysun@ciac.ac.cn
Received Date: 12 January 2018
Revised Date: 9 February 2018
Accepted Date: 26 February 2018
Available Online: 16 April 2018

The dynamic properties of polymer melts are investigated in the range of normal liquid regime to the supercooled liquid regime. The polymer is modeled as a coarse-grained bead-spring model with chain length ranging from 5 to 160. The mean squared displacement and non-Gaussian parameter are used to describe the self diffusion of polymer beads. We find slow dynamics with decreasing temperature and increasing chain length. The time evolution of non-Gaussian parameters shows two peaks (or one peak one shoulder) in the α-relaxation time, τ_α, regime and sub-diffusion time regime, respectively, where the first primary peak indicates the dynamic heterogeneity stemmed from the motion of beads, and the secondary peak is the result of correlated motion along a polymer chain. Moreover, the relaxation of polymer beads shows clear two-step decay in supercooled melts and the dynamics shows growing heterogeneity with decreasing temperature. As chain length is increased, a peak of the dynamic susceptibility occurs, and the peak height, χ \begin{document}$_4^*$\end{document} , increases and then reaches a plateau. The curves of the height of the first peak of \begin{document}$\textit {α}_2^{} $\end{document} , \begin{document}$\textit {α}_2^*$\end{document} , versus \begin{document}$ {\textit {τ}_{\textit {α}}}$\end{document} and the curves of χ \begin{document}$_4^*$\end{document} versus \begin{document}$ {\textit {τ}_{\textit {α}}}$\end{document} follow two master curves for different chain lengths. Our results indicate the similarity of dynamic heterogeneity dominated by the motion of single bead even the chain length is different. It is interesting to find that the Stokes-Einstein (SE) relation between \begin{document}$ {\textit {τ}_{\textit {α}}}$\end{document} and diffusion coefficient D, D~τ \begin{document}${_{q}^{-1}}$\end{document} , is highly length-scale dependent. The SE relation breaks down in both normal melts regime and supercooled regime at large magnitude of wave vectors, attributed to the non-Brownian motion arising from the chain connectivity and growing heterogeneity due to supercooling. However, the SE relation is reconstructed when the probing length scale is large (at small magnitude of wave vectors). Our results show a hierarchical physical picture of the supercooled polymeric dynamics.
- Supercooled polymer melt,
- Molecular dynamics simulation,
- Diffusion,
- Relaxation
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