A theory for heterogeneous states of polymer melts produced by single chain crystal melting

Soft Matter
T C B McLeish

Abstract

We consider the polymer physics of a possible molecular mechanism for disentangled melt states observed recently. We find that the route from molten, but only marginally-overlapping single crystals to the equilibrium state must pass over a free-energy barrier that becomes large at high molecular weights. The penalty arises from elastic distortions of the entanglement network as the chains diffuse. A critical molecular weight arises naturally from the competition of elastic distortion and the free-energy of confinement. We calculate the barrier and critical molecular weight at both a simple single-chain level, and at a "one-loop" level of co-operative motion, finding that many-chain effects alter the physics quantitatively, but not qualitatively. Several new experiments are suggested.

References

Jul 26, 2005·Nature Materials·Sanjay RastogiHans W Spiess

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Citations

Jan 30, 2014·Reports on Progress in Physics·Jonathan D HalversonAlexander Y Grosberg
May 19, 2009·Macromolecular Rapid Communications·Sanjay RastogiPiet J Lemstra
Dec 4, 2017·Polymers·Alper GurarslanAlan E Tonelli
Jun 11, 2021·Soft Matter·Linlin ChuYe-Feng Yao

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