Microscopic dynamics underlying the stress relaxation of arrested soft materials
Abstract
Arrested soft materials such as gels and glasses exhibit a slow stress relaxation with a broad distribution of relaxation times in response to linear mechanical perturbations. Although this macroscopic stress relaxation is an essential feature in the application of arrested systems as structural materials, consumer products, foods, and biological materials, the microscopic origins of this relaxation remain poorly understood. Here, we elucidate the microscopic dynamics underlying the stress relaxation of such arrested soft materials under both quiescent and mechanically perturbed conditions through X-ray photon correlation spectroscopy. By studying the dynamics of a model associative gel system that undergoes dynamical arrest in the absence of aging effects, we show that the mean stress relaxation time measured from linear rheometry is directly correlated to the quiescent superdiffusive dynamics of the microscopic clusters, which are governed by a buildup of internal stresses during arrest. We also show that perturbing the system via small mechanical deformations can result in large intermittent fluctuations in the form of avalanches, which give rise to a broad non-Gaussian spectrum of relaxation modes at short times that is observed in stress relaxation measurements. These findings suggest that the linear viscoelastic stress relaxation in arrested soft materials may be governedmore »
- Authors:
-
[1];
[2];
[4];
[2];
[5];
[6];
[3];
[7]
- Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, MA 01239
- X-ray Sciences Division, Argonne National Laboratory, Lemont, IL 60439
- Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139
- Department of Materials Science and Engineering, North Carolina State University, Raleigh, NC 27695
- Department of Physics, Georgetown University, Washington, DC 20007
- Department of Physics and Astronomy, Johns Hopkins University, Baltimore, MD 21218
- Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, MA 01239
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); US Army Research Laboratory (USARL); US Army Research Office (ARO)
- OSTI Identifier:
- 1876934
- Alternate Identifier(s):
- OSTI ID: 1961606
- Grant/Contract Number:
- Contract # DE-AC02-06CH11357; AC02-06CH11357; CBET-1605943; CBET-1605699; CBET-1804721; DMR-1419807; DMR-2026842; W911NF-13-D-0001
- Resource Type:
- Published Article
- Journal Name:
- Proceedings of the National Academy of Sciences of the United States of America
- Additional Journal Information:
- Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 119 Journal Issue: 30; Journal ID: ISSN 0027-8424
- Publisher:
- Proceedings of the National Academy of Sciences
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; soft materials; stress relaxation; avalanches; gels; viscoelasticity
Citation Formats
Song, Jake, Zhang, Qingteng, de Quesada, Felipe, Rizvi, Mehedi H., Tracy, Joseph B., Ilavsky, Jan, Narayanan, Suresh, Del Gado, Emanuela, Leheny, Robert L., Holten-Andersen, Niels, and McKinley, Gareth H. Microscopic dynamics underlying the stress relaxation of arrested soft materials. United States: N. p., 2022.
Web. doi:10.1073/pnas.2201566119.
Song, Jake, Zhang, Qingteng, de Quesada, Felipe, Rizvi, Mehedi H., Tracy, Joseph B., Ilavsky, Jan, Narayanan, Suresh, Del Gado, Emanuela, Leheny, Robert L., Holten-Andersen, Niels, & McKinley, Gareth H. Microscopic dynamics underlying the stress relaxation of arrested soft materials. United States. https://doi.org/10.1073/pnas.2201566119
Song, Jake, Zhang, Qingteng, de Quesada, Felipe, Rizvi, Mehedi H., Tracy, Joseph B., Ilavsky, Jan, Narayanan, Suresh, Del Gado, Emanuela, Leheny, Robert L., Holten-Andersen, Niels, and McKinley, Gareth H. Tue .
"Microscopic dynamics underlying the stress relaxation of arrested soft materials". United States. https://doi.org/10.1073/pnas.2201566119.
@article{osti_1876934,
title = {Microscopic dynamics underlying the stress relaxation of arrested soft materials},
author = {Song, Jake and Zhang, Qingteng and de Quesada, Felipe and Rizvi, Mehedi H. and Tracy, Joseph B. and Ilavsky, Jan and Narayanan, Suresh and Del Gado, Emanuela and Leheny, Robert L. and Holten-Andersen, Niels and McKinley, Gareth H.},
abstractNote = {Arrested soft materials such as gels and glasses exhibit a slow stress relaxation with a broad distribution of relaxation times in response to linear mechanical perturbations. Although this macroscopic stress relaxation is an essential feature in the application of arrested systems as structural materials, consumer products, foods, and biological materials, the microscopic origins of this relaxation remain poorly understood. Here, we elucidate the microscopic dynamics underlying the stress relaxation of such arrested soft materials under both quiescent and mechanically perturbed conditions through X-ray photon correlation spectroscopy. By studying the dynamics of a model associative gel system that undergoes dynamical arrest in the absence of aging effects, we show that the mean stress relaxation time measured from linear rheometry is directly correlated to the quiescent superdiffusive dynamics of the microscopic clusters, which are governed by a buildup of internal stresses during arrest. We also show that perturbing the system via small mechanical deformations can result in large intermittent fluctuations in the form of avalanches, which give rise to a broad non-Gaussian spectrum of relaxation modes at short times that is observed in stress relaxation measurements. These findings suggest that the linear viscoelastic stress relaxation in arrested soft materials may be governed by nonlinear phenomena involving an interplay of internal stress relaxations and perturbation-induced intermittent avalanches.},
doi = {10.1073/pnas.2201566119},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 30,
volume = 119,
place = {United States},
year = {Tue Jul 19 00:00:00 EDT 2022},
month = {Tue Jul 19 00:00:00 EDT 2022}
}
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