Journal
SCIENCE
Volume 333, Issue 6051, Pages 1871-1874Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1207060
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Funding
- Engineering and Physical Sciences Research Council (UK) under the Microscale Polymer Processing (MuPP) consortium
- European Union under the Marie Curie Initial Training Network Dynamics of Architecturally Complex Polymers
- Engineering and Physical Sciences Research Council [GR/T11807/01, EP/D06631X/1] Funding Source: researchfish
- EPSRC [EP/D06631X/1] Funding Source: UKRI
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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.
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