Abstract
Response to elongational flow is fundamental to soft matter and directly impacts new developments in a broad range of technologies form polymer processing and microfluidics to controlled flow in biosystems. Of particular significance are the effects of elongational flow on self-assembled systems where the interactions between the fundamental building blocks control their adaptation. Here we probe the effects of associating groups on the structure and dynamics of linear polymer melts in uniaxial elongation using molecular dynamics simulations. We study model polymers with randomly incorporated backbone associations with interaction strengths varying from 1kBT to 10kBT. These associating groups drive the formation of clusters in equilibrium with an average size that increases with interaction strength. Flow drives these clusters to continuously break and reform as chains stretch. These flow-driven cluster dynamics drive a qualitative transition in polymer elongation dynamics from homogeneous to nanoscale localized yield and cavitation as the association strength increases.
| Original language | English |
|---|---|
| Article number | 021024 |
| Journal | Physical Review X |
| Volume | 12 |
| Issue number | 2 |
| DOIs | |
| State | Published - Jun 2022 |
| Externally published | Yes |
Funding
D. P. gratefully acknowledges DOE Grant No. DE-SC007908. T. O. gratefully acknowledges startup funding provided by Carnegie Mellon University. The authors kindly acknowledge the use of computational resources provided by NSF No. MRI-1725573. This work was made possible in part by advanced computational resources deployed and maintained by Clemson Computing and Information Technology. This work was supported by the Sandia Laboratory Directed Research and Development Program. This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the U.S. DOE’s National Nuclear Security Administration under Contract No. DENA-0003525. The views expressed in this article do not necessarily represent the views of the U.S. DOE or the U.S. Government.