Topological Methods for Polymeric Materials: Characterizing the Relationship Between Polymer Entanglement and Viscoelasticity

Panagiotou, Eleni; Millett, Kenneth; Atzberger, Paul

doi:10.3390/polym11030437

Topological Methods for Polymeric Materials: Characterizing the Relationship Between Polymer Entanglement and Viscoelasticity

Journal Article · Tue Mar 05 23:00:00 EST 2019 · Polymers

DOI:https://doi.org/10.3390/polym11030437· OSTI ID:1611189

Panagiotou, Eleni ^[1]; Millett, Kenneth ^[2]; ^[2]

Univ. of Tennessee, Chattanooga, TN (United States); DOE/OSTI
Univ. of California, Santa Barbara, CA (United States)

We develop topological methods for characterizing the relationship between polymer chain entanglement and bulk viscoelastic responses. We introduce generalized Linking Number and Writhe characteristics that are applicable to open linear chains. We investigate the rheology of polymeric chains entangled into weaves with varying topologies and levels of chain density. To investigate viscoelastic responses, we perform non-equilibrium molecular simulations over a range of frequencies using sheared Lees–Edwards boundary conditions. We show how our topological characteristics can be used to capture key features of the polymer entanglements related to the viscoelastic responses. We find there is a linear relation over a significant range of frequencies between the mean absolute Writhe W r and the Loss Tangent tan ( δ ) . We also find an approximate inverse linear relationship between the mean absolute Periodic Linking Number L K P and the Loss Tangent tan ( δ ) . Our results show some of the ways topological methods can be used to characterize chain entanglements to better understand the origins of mechanical responses in polymeric materials.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of California, Santa Barbara, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR) (SC-21)

Grant/Contract Number:: SC0009254

OSTI ID:: 1611189

Journal Information:: Polymers, Journal Name: Polymers Journal Issue: 3 Vol. 11; ISSN POLYCK; ISSN 2073-4360

Publisher:: MDPICopyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
97 MATHEMATICS AND COMPUTING
Polymer Science
entanglements
knots
linking number
oscillatory shear
topology
viscoelasticity
writhe

Topological Methods for Polymeric Materials: Characterizing the Relationship Between Polymer Entanglement and Viscoelasticity

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References (73)

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