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Revisiting the concept of activation in supercooled liquids

In this work, we revisit the description of dynamics based on the concepts of metabasins and activation in mildly supercooled liquids via the analysis of the dynamics of a paradigmatic glass former between its onset temperature [Formula: see text] and mode-coupling temperature [Formula: see text] ....

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Autores principales: Baity-Jesi, Marco, Biroli, Giulio, Reichman, David R.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Springer Berlin Heidelberg 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8203548/
https://www.ncbi.nlm.nih.gov/pubmed/34125327
http://dx.doi.org/10.1140/epje/s10189-021-00077-y
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author Baity-Jesi, Marco
Biroli, Giulio
Reichman, David R.
author_facet Baity-Jesi, Marco
Biroli, Giulio
Reichman, David R.
author_sort Baity-Jesi, Marco
collection PubMed
description In this work, we revisit the description of dynamics based on the concepts of metabasins and activation in mildly supercooled liquids via the analysis of the dynamics of a paradigmatic glass former between its onset temperature [Formula: see text] and mode-coupling temperature [Formula: see text] . First, we provide measures that demonstrate that the onset of glassiness is indeed connected to the landscape, and that metabasin waiting time distributions are so broad that the system can remain stuck in a metabasin for times that exceed [Formula: see text] by orders of magnitude. We then reanalyze the transitions between metabasins, providing several indications that the standard picture of activated dynamics in terms of traps does not hold in this regime. Instead, we propose that here activation is principally driven by entropic instead of energetic barriers. In particular, we illustrate that activation is not controlled by the hopping of high energetic barriers and should more properly be interpreted as the entropic selection of nearly barrierless but rare pathways connecting metabasins on the landscape.
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spelling pubmed-82035482021-06-17 Revisiting the concept of activation in supercooled liquids Baity-Jesi, Marco Biroli, Giulio Reichman, David R. Eur Phys J E Soft Matter Regular Article - Flowing Matter In this work, we revisit the description of dynamics based on the concepts of metabasins and activation in mildly supercooled liquids via the analysis of the dynamics of a paradigmatic glass former between its onset temperature [Formula: see text] and mode-coupling temperature [Formula: see text] . First, we provide measures that demonstrate that the onset of glassiness is indeed connected to the landscape, and that metabasin waiting time distributions are so broad that the system can remain stuck in a metabasin for times that exceed [Formula: see text] by orders of magnitude. We then reanalyze the transitions between metabasins, providing several indications that the standard picture of activated dynamics in terms of traps does not hold in this regime. Instead, we propose that here activation is principally driven by entropic instead of energetic barriers. In particular, we illustrate that activation is not controlled by the hopping of high energetic barriers and should more properly be interpreted as the entropic selection of nearly barrierless but rare pathways connecting metabasins on the landscape. Springer Berlin Heidelberg 2021-06-14 2021 /pmc/articles/PMC8203548/ /pubmed/34125327 http://dx.doi.org/10.1140/epje/s10189-021-00077-y Text en © The Author(s) 2021 https://creativecommons.org/licenses/by/4.0/Open AccessThis 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 licence, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence 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 licence, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Regular Article - Flowing Matter
Baity-Jesi, Marco
Biroli, Giulio
Reichman, David R.
Revisiting the concept of activation in supercooled liquids
title Revisiting the concept of activation in supercooled liquids
title_full Revisiting the concept of activation in supercooled liquids
title_fullStr Revisiting the concept of activation in supercooled liquids
title_full_unstemmed Revisiting the concept of activation in supercooled liquids
title_short Revisiting the concept of activation in supercooled liquids
title_sort revisiting the concept of activation in supercooled liquids
topic Regular Article - Flowing Matter
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8203548/
https://www.ncbi.nlm.nih.gov/pubmed/34125327
http://dx.doi.org/10.1140/epje/s10189-021-00077-y
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