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Berlin 2015 – scientific programme

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CPP: Fachverband Chemische Physik und Polymerphysik

CPP 8: Colloids and Complex Liquids II (joint session CPP, BP, DY)

CPP 8.14: Talk

Monday, March 16, 2015, 18:30–18:45, C 130

Excess entropy scaling for the segmental and global dynamics of polyethylene melts — •Evangelos Voyiatzis, Michael Böhm, and Florian Müller-Plathe — Eduard-Zintl-Institut für Anorganische und Physikalische Chemie and Center of Smart Interfaces, Technische Universität Darmstadt, Alarich-Weiss-Strasse 4, D-64287 Darmstadt, Germany

The range of validity of the Rosenfeld and Dzugutov excess entropy scaling laws is analyzed for linear polyethylene chains. We consider two segmental dynamical quantities, the bond and the torsional relaxation times, and two global ones, the chain diffusion coefficient and the viscosity. The excess entropy is approximated by either a series expansion of the entropy in terms of the pair correlation function or by an equation of state for polymers. For all temperatures and chain lengths considered, the two excess entropy estimates are linearly correlated. The scaled segmental relaxation times fall into a non-linear master curve. For a fixed chain length, the reduced diffusion coefficient and viscosity scale linearly with the excess entropy. An empirical reduction to a chain length independent master curve is accessible for both quantities. The Dzugutov scheme predicts an increased value of the scaled diffusion coefficient with increasing chain length which contrasts physical expectations. The origin of this trend can be traced back to the density dependence of the scaling factors. In connection with diffusion coefficients and viscosities, the Rosenfeld scaling appears to be of higher quality than the Dzugutov. An empirical excess entropy scaling is also proposed which leads to a chain length-independent correlation.

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