Linking Models of Polymerization and Dynamics to Predict Branched Polymer Structure and Flow

Read, Daniel J.; Auhl, Dietmar; Das, Chinmay; den Doelder, Jaap; Kapnistos, Michael; Vittorias, Iakovos; McLeish, Tom C.B.

doi:10.1126/science.1207060

Linking Models of Polymerization and Dynamics to Predict Branched Polymer Structure and Flow

Read, Daniel J.; Auhl, Dietmar; Das, Chinmay; den Doelder, Jaap; Kapnistos, Michael; Vittorias, Iakovos; McLeish, Tom C.B.

Authors

Daniel J. Read

Dietmar Auhl

Chinmay Das

Jaap den Doelder

Michael Kapnistos

Iakovos Vittorias

Tom C.B. McLeish

Abstract

We present a predictive scheme connecting the topological structure of highly branched entangled polymers, with industrial-level complexity, to the emergent viscoelasticity of the polymer melt. The scheme is able to calculate the linear and nonlinear viscoelasticity of a stochastically branched “high-pressure free radical” polymer melt as a function of the chemical kinetics of its formation. The method combines numerical simulation of polymerization with the tube/entanglement physics of polymer dynamics extended to fully nonlinear response. We compare calculations for a series of low-density polyethylenes with experiments on structural and viscoelastic properties. The method provides a window onto the molecular processes responsible for the optimized rheology of these melts, connecting fundamental science to process in complex flow, and opens up the in silico design of new materials.

Citation

Read, D. J., Auhl, D., Das, C., den Doelder, J., Kapnistos, M., Vittorias, I., & McLeish, T. C. (2011). Linking Models of Polymerization and Dynamics to Predict Branched Polymer Structure and Flow. Science, 333(6051), 1871-1874. https://doi.org/10.1126/science.1207060

Journal Article Type	Article
Publication Date	Sep 1, 2011
Deposit Date	Jan 21, 2013
Publicly Available Date	Jan 23, 2013
Journal	Science
Print ISSN	0036-8075
Electronic ISSN	1095-9203
Publisher	American Association for the Advancement of Science
Peer Reviewed	Peer Reviewed
Volume	333
Issue	6051
Pages	1871-1874
DOI	https://doi.org/10.1126/science.1207060

Files

Accepted Journal Article (595 Kb)
PDF

Copyright Statement
This is the author's version of the work. It is posted here by permission of the AAAS for personal use, not for redistribution. The definitive version was published in Science 333/6051, http://dx.doi.org/10.1126/science.1207060