Temperature dependent micro-rheology of a glass-forming polymer melt studied by molecular dynamics simulation

We present a Molecular Dynamics simulation study of a micro-rheological probing of the glass transition in a polymer melt. Our model system consists of short bead-spring chains and the temperature ranges from well above the glass transition temperature to about 10% above it. The nano-particle clearly couples to the slowing down of the polymer segments and the calculated storage and loss moduli reveal the approach to the glass transition. At temperatures close to the mode coupling T-c of the polymer melt, the micro-rheological moduli measure the local viscoelastic response of the cage of monomers surrounding the nano-particle and no longer reveal the true melt moduli. The incoherent scattering function of the nano-particle exhibits a stretched exponential decay, typical for the alpha-process in glass forming systems. We find no indication of a strong superdiffusive regime as has been deduced from a recent experiment in the same temperature range but for smaller momentum transfers. (C) 2014 AIP Publishing LLC.