Energy renormalization approach to coarse-graining of polymer dynamics

Published

August 8, 2017

Author(s)

Wenjie Xia, Jake Song, Cheol Jeong, David D. Hsu, Frederick R. Phelan Jr., Jack F. Douglas, Sinan Keten

Abstract

A major challenge in soft matter science is the bottom-up prediction of the temperature- dependent behavior of amorphous glass-forming (GF) polymers. Coarse-grained (CG) models derived from atomistic simulation data offer chemical specificity and access to relevant time-scales, but exhibit faster dynamics due to their reduced degrees of freedom. Based on the common notion of a temperature-dependent activation energy in glass formation theories, we find that renormalizing the CG cohesive energy parameters as a sigmoidal function of temperature allows accurate prediction of atomistic polymer dynamics over the Arrhenius regime, the non-Arrhenius regime of incipient of glass-formation and the glassy state. We establish a systematic approach to enthalpically compensate for the altered configurational entropy and cooperatively rearranging regions (CRRs) in CG modeling. This represents critical progress for building temperature-transferable CG models that predict key properties of GF polymer materials. The unique role that cohesive interactions play on GF characteristics as highlighted in this work reveals new opportunities for the tailored design of GF polymer materials.

Citation

Macromolecules

Volume

50

Issue

21

Pub Type

Journals

Download Paper

https://doi.org/10.1021/acs.macromol.7b01717

Keywords

coarse-grained modeling, polymer dynamics, polymer glass, molecular dynamics

Citation

Xia, W. , Song, J. , Jeong, C. , Hsu, D. , Phelan, F. , Douglas, J. and Keten, S. (2017), Energy renormalization approach to coarse-graining of polymer dynamics, Macromolecules, [online], https://doi.org/10.1021/acs.macromol.7b01717 (Accessed October 9, 2025)