Glassy Dynamics of Simulated Polymer Melts: Coherent Scattering and Van Hove Correlation Functions Part I: Dynamics in the beta-Relaxation Regime

Abstract

We report results of molecular-dynamics simulations of a model polymer melt consisting of short non-entangled chains in the supercooled state above the critical temperature of mode-coupling theory (MCT). To analyse the dynamics of the system we computed the incoherent, collective chain and melt intermediate scattering functions as well as the Van Hove correlation functions. We find good evidence for the space-time factorization theorem of MCT. From the critical amplitudes we could derive typical length scales of the beta-dyamics. In an extensive quantitative analysis the leading order description of MCT was found to be accurate in the central beta-regime. Higher order corrections extend the validity of the MCT approximation to a greater time window. Indications of polymer specific effects on the length scale of the chain's radius of gyration are visible in the beta-coefficients.