Scale-free center-of-mass displacement correlations in dense polymer solutions and melts without topological constraints and momentum conservation: A bond-fluctuation model study

Details Scale-free center-of-mass displacement correlations in dense polymer solutions and melts without topological constraints and momentum conservation: A bond-fluctuation model study Scale-free center-of-mass displacement correlations in dense polymer solutions and melts without topological constraints and momentum conservation: A bond-fluctuation model study

2011-02-24

arxiv.org/abs/1102.4962v2

Physics

Condensed Matter

Soft Condensed Matter

27 pages, 12 figures

Scientific paper

By Monte Carlo simulations of a variant of the bond-fluctuation model without topological constraints we examine the center-of-mass (COM) dynamics of polymer melts in $d=3$ dimensions. Our analysis focuses on the COM displacement correlation function $\CN(t) \approx \partial_t^2 \MSDcmN(t)/2$, measuring the curvature of the COM mean-square displacement $\MSDcmN(t)$. We demonstrate that $\CN(t) \approx -(\RN/\TN)^2 (\rhostar/\rho) \ f(x=t/\TN)$ with $N$ being the chain length ($16 \le N \le 8192$), $\RN\sim N^{1/2}$ the typical chain size, $\TN\sim N^2$ the longest chain relaxation time, $\rho$ the monomer density, $\rhostar \approx N/\RN^d$ the self-density and $f(x)$ a universal function decaying asymptotically as $f(x) \sim x^{-\omega}$ with $\omega = (d+2) \times \alpha$ where $\alpha = 1/4$ for $x \ll 1$ and $\alpha = 1/2$ for $x \gg 1$. We argue that the algebraic decay $N \CN(t) \sim - t^{-5/4}$ for $t \ll \TN$ results from an interplay of chain connectivity and melt incompressibility giving rise to the correlated motion of chains and subchains.

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