Time–connectivity superposition and the gel/glass duality of weak colloidal gels

Colloidal gels result from the aggregation of Brownian particles suspended in a solvent. Gelation is induced by attractive interactions between individual particles that drive the formation of clusters, which in turn aggregate to form a space-spanning structure. We study this process in aluminosilic...

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Main Authors: Keshavarz, Bavand, Rodrigues, Donatien Gomes, Champenois, Jean-Baptiste, Frith, Matthew G, Ilavsky, Jan, Geri, Michela, Divoux, Thibaut, McKinley, Gareth H, Poulesquen, Arnaud
Other Authors: Massachusetts Institute of Technology. Department of Mechanical Engineering
Format: Article
Language:English
Published: Proceedings of the National Academy of Sciences 2022
Online Access:https://hdl.handle.net/1721.1/138880
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author Keshavarz, Bavand
Rodrigues, Donatien Gomes
Champenois, Jean-Baptiste
Frith, Matthew G
Ilavsky, Jan
Geri, Michela
Divoux, Thibaut
McKinley, Gareth H
Poulesquen, Arnaud
author2 Massachusetts Institute of Technology. Department of Mechanical Engineering
author_facet Massachusetts Institute of Technology. Department of Mechanical Engineering
Keshavarz, Bavand
Rodrigues, Donatien Gomes
Champenois, Jean-Baptiste
Frith, Matthew G
Ilavsky, Jan
Geri, Michela
Divoux, Thibaut
McKinley, Gareth H
Poulesquen, Arnaud
author_sort Keshavarz, Bavand
collection MIT
description Colloidal gels result from the aggregation of Brownian particles suspended in a solvent. Gelation is induced by attractive interactions between individual particles that drive the formation of clusters, which in turn aggregate to form a space-spanning structure. We study this process in aluminosilicate colloidal gels through time-resolved structural and mechanical spectroscopy. Using the time–connectivity superposition principle a series of rapidly acquired linear viscoelastic spectra, measured throughout the gelation process by applying an exponential chirp protocol, are rescaled onto a universal master curve that spans over eight orders of magnitude in reduced frequency. This analysis reveals that the underlying relaxation time spectrum of the colloidal gel is symmetric in time with power-law tails characterized by a single exponent that is set at the gel point. The microstructural mechanical network has a dual character; at short length scales and fast times it appears glassy, whereas at longer times and larger scales it is gel-like. These results can be captured by a simple three-parameter constitutive model and demonstrate that the microstructure of a mature colloidal gel bears the residual skeleton of the original sample-spanning network that is created at the gel point. Our conclusions are confirmed by applying the same technique to another well-known colloidal gel system composed of attractive silica nanoparticles. The results illustrate the power of the time–connectivity superposition principle for this class of soft glassy materials and provide a compact description for the dichotomous viscoelastic nature of weak colloidal gels.
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spelling mit-1721.1/1388802023-04-14T19:38:31Z Time–connectivity superposition and the gel/glass duality of weak colloidal gels Keshavarz, Bavand Rodrigues, Donatien Gomes Champenois, Jean-Baptiste Frith, Matthew G Ilavsky, Jan Geri, Michela Divoux, Thibaut McKinley, Gareth H Poulesquen, Arnaud Massachusetts Institute of Technology. Department of Mechanical Engineering MultiScale Materials Science for Energy and Environment, Joint MIT-CNRS Laboratory Colloidal gels result from the aggregation of Brownian particles suspended in a solvent. Gelation is induced by attractive interactions between individual particles that drive the formation of clusters, which in turn aggregate to form a space-spanning structure. We study this process in aluminosilicate colloidal gels through time-resolved structural and mechanical spectroscopy. Using the time–connectivity superposition principle a series of rapidly acquired linear viscoelastic spectra, measured throughout the gelation process by applying an exponential chirp protocol, are rescaled onto a universal master curve that spans over eight orders of magnitude in reduced frequency. This analysis reveals that the underlying relaxation time spectrum of the colloidal gel is symmetric in time with power-law tails characterized by a single exponent that is set at the gel point. The microstructural mechanical network has a dual character; at short length scales and fast times it appears glassy, whereas at longer times and larger scales it is gel-like. These results can be captured by a simple three-parameter constitutive model and demonstrate that the microstructure of a mature colloidal gel bears the residual skeleton of the original sample-spanning network that is created at the gel point. Our conclusions are confirmed by applying the same technique to another well-known colloidal gel system composed of attractive silica nanoparticles. The results illustrate the power of the time–connectivity superposition principle for this class of soft glassy materials and provide a compact description for the dichotomous viscoelastic nature of weak colloidal gels. 2022-01-11T17:49:17Z 2022-01-11T17:49:17Z 2021 2022-01-11T17:38:50Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/138880 Keshavarz, Bavand, Rodrigues, Donatien Gomes, Champenois, Jean-Baptiste, Frith, Matthew G, Ilavsky, Jan et al. 2021. "Time–connectivity superposition and the gel/glass duality of weak colloidal gels." Proceedings of the National Academy of Sciences of the United States of America, 118 (15). en 10.1073/PNAS.2022339118 Proceedings of the National Academy of Sciences of the United States of America Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf Proceedings of the National Academy of Sciences PNAS
spellingShingle Keshavarz, Bavand
Rodrigues, Donatien Gomes
Champenois, Jean-Baptiste
Frith, Matthew G
Ilavsky, Jan
Geri, Michela
Divoux, Thibaut
McKinley, Gareth H
Poulesquen, Arnaud
Time–connectivity superposition and the gel/glass duality of weak colloidal gels
title Time–connectivity superposition and the gel/glass duality of weak colloidal gels
title_full Time–connectivity superposition and the gel/glass duality of weak colloidal gels
title_fullStr Time–connectivity superposition and the gel/glass duality of weak colloidal gels
title_full_unstemmed Time–connectivity superposition and the gel/glass duality of weak colloidal gels
title_short Time–connectivity superposition and the gel/glass duality of weak colloidal gels
title_sort time connectivity superposition and the gel glass duality of weak colloidal gels
url https://hdl.handle.net/1721.1/138880
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