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Soft pinning: Experimental validation of static correlations in supercooled molecular glass-forming liquids

Enormous enhancement in the viscosity of a liquid near its glass transition is a hallmark of glass transition. Within a class of theoretical frameworks, it is connected to growing many-body static correlations near the transition, often called “amorphous ordering.” At the same time, some theories do...

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Autores principales: Das, Rajsekhar, Bhowmik, Bhanu Prasad, Puthirath, Anand B, Narayanan, Tharangattu N, Karmakar, Smarajit
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Oxford University Press 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10482383/
https://www.ncbi.nlm.nih.gov/pubmed/37680690
http://dx.doi.org/10.1093/pnasnexus/pgad277
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author Das, Rajsekhar
Bhowmik, Bhanu Prasad
Puthirath, Anand B
Narayanan, Tharangattu N
Karmakar, Smarajit
author_facet Das, Rajsekhar
Bhowmik, Bhanu Prasad
Puthirath, Anand B
Narayanan, Tharangattu N
Karmakar, Smarajit
author_sort Das, Rajsekhar
collection PubMed
description Enormous enhancement in the viscosity of a liquid near its glass transition is a hallmark of glass transition. Within a class of theoretical frameworks, it is connected to growing many-body static correlations near the transition, often called “amorphous ordering.” At the same time, some theories do not invoke the existence of such a static length scale in the problem. Thus, proving the existence and possible estimation of the static length scales of amorphous order in different glass-forming liquids is very important to validate or falsify the predictions of these theories and unravel the true physics of glass formation. Experiments on molecular glass-forming liquids become pivotal in this scenario as the viscosity grows several folds ([Formula: see text]), and simulations or colloidal glass experiments fail to access these required long-time scales. Here we design an experiment to extract the static length scales in molecular liquids using dilute amounts of another large molecule as a pinning site. Results from dielectric relaxation experiments on supercooled Glycerol with different pinning concentrations of Sorbitol and Glucose, as well as the simulations on a few model glass-forming liquids with pinning sites, indicate the versatility of the proposed method, opening possible new avenues to study the physics of glass transition in other molecular liquids.
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spelling pubmed-104823832023-09-07 Soft pinning: Experimental validation of static correlations in supercooled molecular glass-forming liquids Das, Rajsekhar Bhowmik, Bhanu Prasad Puthirath, Anand B Narayanan, Tharangattu N Karmakar, Smarajit PNAS Nexus Physical Sciences and Engineering Enormous enhancement in the viscosity of a liquid near its glass transition is a hallmark of glass transition. Within a class of theoretical frameworks, it is connected to growing many-body static correlations near the transition, often called “amorphous ordering.” At the same time, some theories do not invoke the existence of such a static length scale in the problem. Thus, proving the existence and possible estimation of the static length scales of amorphous order in different glass-forming liquids is very important to validate or falsify the predictions of these theories and unravel the true physics of glass formation. Experiments on molecular glass-forming liquids become pivotal in this scenario as the viscosity grows several folds ([Formula: see text]), and simulations or colloidal glass experiments fail to access these required long-time scales. Here we design an experiment to extract the static length scales in molecular liquids using dilute amounts of another large molecule as a pinning site. Results from dielectric relaxation experiments on supercooled Glycerol with different pinning concentrations of Sorbitol and Glucose, as well as the simulations on a few model glass-forming liquids with pinning sites, indicate the versatility of the proposed method, opening possible new avenues to study the physics of glass transition in other molecular liquids. Oxford University Press 2023-08-25 /pmc/articles/PMC10482383/ /pubmed/37680690 http://dx.doi.org/10.1093/pnasnexus/pgad277 Text en © The Author(s) 2023. Published by Oxford University Press on behalf of National Academy of Sciences. https://creativecommons.org/licenses/by/4.0/This is an Open Access article distributed under the terms of the Creative Commons Attribution License (https://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse, distribution, and reproduction in any medium, provided the original work is properly cited.
spellingShingle Physical Sciences and Engineering
Das, Rajsekhar
Bhowmik, Bhanu Prasad
Puthirath, Anand B
Narayanan, Tharangattu N
Karmakar, Smarajit
Soft pinning: Experimental validation of static correlations in supercooled molecular glass-forming liquids
title Soft pinning: Experimental validation of static correlations in supercooled molecular glass-forming liquids
title_full Soft pinning: Experimental validation of static correlations in supercooled molecular glass-forming liquids
title_fullStr Soft pinning: Experimental validation of static correlations in supercooled molecular glass-forming liquids
title_full_unstemmed Soft pinning: Experimental validation of static correlations in supercooled molecular glass-forming liquids
title_short Soft pinning: Experimental validation of static correlations in supercooled molecular glass-forming liquids
title_sort soft pinning: experimental validation of static correlations in supercooled molecular glass-forming liquids
topic Physical Sciences and Engineering
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10482383/
https://www.ncbi.nlm.nih.gov/pubmed/37680690
http://dx.doi.org/10.1093/pnasnexus/pgad277
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