Molecular-dynamics simulation of a glassy polymer melt: Incoherent scattering function
Institut für Physik, Johannes-Gutenberg Universität,
Staudinger Weg 7, 55099 Mainz, Germany
Corresponding author: a Joerg.Baschnagel@uni-mainz.de
Published online: 15 July 1999
We present simulation results for a model polymer melt, consisting of short, nonentangled chains, in the supercooled state. The analysis focuses on the monomer dynamics, which is monitored by the incoherent intermediate scattering function. The scattering function is recorded over six decades in time and for many different wave-vectors which range from the size of a chain to about three times the maximum position of the static structure factor. The lowest temperatures studied are slightly above , the critical temperature of mode-coupling theory (MCT), where was determined from a quantitative analysis of the β- and α-relaxations. We find evidence for the space-time factorization theorem in the β-relaxation regime, and for the time-temperature superposition principle in the α-regime, if the temperature is not too close to . The wave-vector (q-) dependence of the nonergodicity parameter, of the critical amplitude, and the α-relaxation time are in qualitative agreement with calculations for hard spheres. For q larger than the maximum of the structure factor the α-relaxation time already agrees fairly well with the asymptotic MCT-prediction . The behavior of the relaxation time at small q can be rationalized by the validity of the Gaussian approximation and the value of the Kohlrausch stretching exponent, as suggested in neutron-scattering experiments.
PACS: 61.20.Ja – Computer simulation of liquid structure / 64.70.Pf – Glass transitions / 61.25.Hq – Macromolecular and polymer solutions; polymer melts; swelling
© EDP Sciences, Società Italiana di Fisica, Springer-Verlag, 1999