Abstract
Conditions of rapid processing often drive polymers to adopt nonequilibrium molecular conformations, which, in turn, can give rise to structural, dynamical, and mechanical properties that are significantly different from those in thermodynamic equilibrium. However, despite the possibility to control the desired nonequilibrium properties of polymers, a rigorous microscopic understanding of the processing-property relations is currently lacking. In an attempt to stimulate progress along this topical direction, we focus here on three prototypical and apparently different cases: spin-coated polymer films, rapidly drawn polymer fibers, and sheared polymer melts. Inspired by the presence of common observations in the chosen cases, we search for order parameters as, for example, topological correlations and heterogeneities, which may allow characterizing the processing-induced behavior of polymers. We highlight that such approaches, necessitating concerted efforts from theory, simulations, and experiments, can provide a profound understanding leading to predictable and tunable properties of polymers.
| Original language | English |
|---|---|
| Pages (from-to) | 7146-7156 |
| Number of pages | 11 |
| Journal | Macromolecules |
| Volume | 52 |
| Issue number | 19 |
| DOIs | |
| Publication status | Published - Aug 2019 |
Funding
Liesbeth M. C. Janssen is Assistant Professor in the department of Applied Physics at Eindhoven University of Technology, The Netherlands. She studied Chemistry at Radboud University Nijmegen and obtained her PhD in Theoretical Chemistry from the same university in 2012. Following postdoctoral stays at Columbia University, New York, working with Prof. David Reichman, and Heinrich-Heine University Düsseldorf, working with Prof. Hartmut Löwen, she established her own group in Eindhoven in 2017. Her research focuses on theory and simulation of nonequilibrium soft matter, including glass-forming materials and polymers, active matter, and glassy biological systems. In 2016, she was the recipient of the Mildred Dresselhaus Award and Guest Professorship at CUI, Hamburg. Her research has been supported by several personal fellowships, including an NWO Rubicon fellowship, Alexander von Humboldt research fellowship, and NWO START-UP grant. Jun Xu is now an associate professor in Department of Chemical Engineering, Tsinghua University. He obtained his B.Sc. and Ph.D. degree at the Department of Chemical Engineering, Tsinghua University in 1997 and 2002, respectively. He was awarded the Alexander von Humboldt Research Fellowship for Experienced Researchers in 2011 and Feng Xingde Polymer Prize for winning “The Best Paper Nomination from China” published in the journal of Polymer in 2011. He was supported by the Program for New Century Excellent Talents in University in 2012. His research interests are in the field of polymer crystallization, biodegradable polymers, bioinspired materials, self-healing and recyclable polymers, 3-D printing, and so on. His work has revealed the twisting process of lamellar crystals in the polymer banded spherulites and what directs the twisting sense. He is now focusing on the nucleation mechanism of polymer lamellar crystals via combining theory and experiments. Simone Napolitano studied Materials Science at the Università di Pisa and received his PhD in Polymer Physics from KULeuven in 2008 and went on to complete postdoctoral work at the Research Foundation Flanders (FWO). In 2011, he joined the Université libre de Bruxelles (ULB). There he serves the Faculty of Science as associate professor and leads the Laboratory of Polymers and Soft Matter Dynamics and the group of Experimental Soft Matter and Thermal Physics. His research focuses on the molecular origin of the glass transition and the correlation between structure and dynamics in polymers and small molecules under nanoscopic confinement. His group is currently working on the physics of irreversible adsorption and on nonequilibrium phenomena in confined soft matter. This work is an outcome of stimulating and intensive discussions among the authors, searching for a unifying approach to understand a wide spectrum of largely unexpected, variable, and novel properties of polymers. We acknowledge the funding support from the International Research Training Group (IRTG-1642) - Soft Matter Science, funded by the Deutsche Forschunggemeinschaft (DFG). S.C. acknowledges funding support from DFG via CH 1741/2-1. U.S. acknowledges partial funding from the Adolphe Merkle Foundation.