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Experimental evidence of mosaic structure in strongly supercooled molecular liquids

When a liquid is cooled to produce a glass its dynamics, dominated by the structural relaxation, become very slow, and at the glass-transition temperature T(g) its characteristic relaxation time is about 100 s. At slightly elevated temperatures (~1.2 T(g)) however, a second process known as the Joha...

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Autores principales: Caporaletti, F., Capaccioli, S., Valenti, S., Mikolasek, M., Chumakov, A. I., Monaco, G.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7994800/
https://www.ncbi.nlm.nih.gov/pubmed/33767148
http://dx.doi.org/10.1038/s41467-021-22154-8
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author Caporaletti, F.
Capaccioli, S.
Valenti, S.
Mikolasek, M.
Chumakov, A. I.
Monaco, G.
author_facet Caporaletti, F.
Capaccioli, S.
Valenti, S.
Mikolasek, M.
Chumakov, A. I.
Monaco, G.
author_sort Caporaletti, F.
collection PubMed
description When a liquid is cooled to produce a glass its dynamics, dominated by the structural relaxation, become very slow, and at the glass-transition temperature T(g) its characteristic relaxation time is about 100 s. At slightly elevated temperatures (~1.2 T(g)) however, a second process known as the Johari-Goldstein relaxation, β(JG), decouples from the structural one and remains much faster than it down to T(g). While it is known that the β(JG)-process is strongly coupled to the structural relaxation, its dedicated role in the glass-transition remains under debate. Here we use an experimental technique that permits us to investigate the spatial and temporal properties of the β(JG) relaxation, and give evidence that the molecules participating in it are highly mobile and spatially connected in a system-spanning, percolating cluster. This correlation of structural and dynamical properties provides strong experimental support for a picture, drawn from theoretical studies, of an intermittent mosaic structure in the deeply supercooled liquid phase.
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spelling pubmed-79948002021-04-16 Experimental evidence of mosaic structure in strongly supercooled molecular liquids Caporaletti, F. Capaccioli, S. Valenti, S. Mikolasek, M. Chumakov, A. I. Monaco, G. Nat Commun Article When a liquid is cooled to produce a glass its dynamics, dominated by the structural relaxation, become very slow, and at the glass-transition temperature T(g) its characteristic relaxation time is about 100 s. At slightly elevated temperatures (~1.2 T(g)) however, a second process known as the Johari-Goldstein relaxation, β(JG), decouples from the structural one and remains much faster than it down to T(g). While it is known that the β(JG)-process is strongly coupled to the structural relaxation, its dedicated role in the glass-transition remains under debate. Here we use an experimental technique that permits us to investigate the spatial and temporal properties of the β(JG) relaxation, and give evidence that the molecules participating in it are highly mobile and spatially connected in a system-spanning, percolating cluster. This correlation of structural and dynamical properties provides strong experimental support for a picture, drawn from theoretical studies, of an intermittent mosaic structure in the deeply supercooled liquid phase. Nature Publishing Group UK 2021-03-25 /pmc/articles/PMC7994800/ /pubmed/33767148 http://dx.doi.org/10.1038/s41467-021-22154-8 Text en © The Author(s) 2021 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Caporaletti, F.
Capaccioli, S.
Valenti, S.
Mikolasek, M.
Chumakov, A. I.
Monaco, G.
Experimental evidence of mosaic structure in strongly supercooled molecular liquids
title Experimental evidence of mosaic structure in strongly supercooled molecular liquids
title_full Experimental evidence of mosaic structure in strongly supercooled molecular liquids
title_fullStr Experimental evidence of mosaic structure in strongly supercooled molecular liquids
title_full_unstemmed Experimental evidence of mosaic structure in strongly supercooled molecular liquids
title_short Experimental evidence of mosaic structure in strongly supercooled molecular liquids
title_sort experimental evidence of mosaic structure in strongly supercooled molecular liquids
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7994800/
https://www.ncbi.nlm.nih.gov/pubmed/33767148
http://dx.doi.org/10.1038/s41467-021-22154-8
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