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Quantitative Model for Clusters of String-like Cooperative Motion in a Coarse-Grained Glass-Forming Polymer Melt

Published online by Cambridge University Press:  30 January 2014

Beatriz A Pazmiño Betancourt ,
Jack F. Douglas  and
Francis W. Starr
Beatriz A Pazmiño Betancourt
Affiliation:
Department of Physics, Wesleyan University, Middletown, Connecticut 06459, USA
Jack F. Douglas
Affiliation:
Materials Science and Engineering, National Institute of Standards and Technology, Gaithersburg, Maryland, 20899.
Francis W. Starr
Affiliation:
Department of Physics, Wesleyan University, Middletown, Connecticut 06459, USA
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Abstract

We apply a living polymerization theory to describe cooperative string-like particle rearrangement clusters observed in simulations of a coarse-grained polymer melt. The theory quantitatively describes the interrelation between the average string length L, configurational entropy Sconf, and the order parameter for string assembly Φ without free parameters. Combining this theory with the Adam-Gibbs (AG) model allows us to predict the relaxation time τ in a lower temperature T range than accessible by current simulations. In particular, the combined theories suggest a return to Arrhenius behavior near Tg and a low T residual entropy, thus avoiding a Kauzmann ‘entropy crisis’.

Keywords

simulationpolymerself-assembly
Type
Articles
Information
MRS Online Proceedings Library (OPL) , Volume 1622: Symposium E – Fundamentals of Gels and Self-Assembled Polymer Systems , 2014 , pp. 95 - 111
Copyright
Copyright © Materials Research Society 2014 

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