Organic Glass-Forming Liquids and the Concept of Fragility

Christiane Alba-Simionesco

doi:10.5802/crphys.148

Organic Glass-Forming Liquids and the Concept of Fragility

Christiane Alba-Simionesco ¹

¹ Laboratoire Léon Brillouin, Université Paris-Saclay, CEA, CNRS, 91191, Gif-sur-Yvette, France

Comptes Rendus. Physique, From everyday glass to disordered solids, Volume 24 (2023) no. S1, pp. 177-198.

Abstract
Résumé

An important category of glass-forming materials is organic; it includes molecular liquids, polymers, solutions, proteins that can be vitrified by cooling the liquid under standard conditions or after special thermal treatments. The range of applications is large from materials to life sciences and recently to electronics. To distinguish them from other systems described in this issue, some specific properties such as the range of their glass transition temperature ( $T_{g}$ ), their ability to vitrify and some rules of thumb to locate $T_{g}$ are presented. The most remarkable property of these liquids is how fast in temperature their viscosity or structural relaxation time increases as approaching $T_{g}$ . To characterize this behavior and rank the liquids of different strength, C.A. Angell introduced the concept of Fragility nearly $40$ years ago. He proposed to classify liquids as fragile or strong in an Arrhenius plot with $T_{g}$ scaling (the strongest ones have never being observed in organic glasses, except for water under specific conditions). The $T_{g}$ value and the fragility index of a given liquid can be changed by applying pressure, i.e. changing the density. One can then explore the properties of the supercooled/overcompressed liquid and the glass in a $P - T$ phase diagram. The $T_{g}$ line corresponds to an isochronic line, i.e. a line at constant relaxation time for different pairs of density-temperature. We observe that all data can be placed on master-curves that depend only on a single density- and species-dependent and T-independent effective interaction energy, $E_{\infty} (ρ)$ . An isochoric fragility index is defined as an intrinsic property of a given liquid, that can help in rationalizing all the correlations between the glass properties below $T_{g}$ and the viscous slowing down just above $T_{g}$ from which they are made. Geometrical confinement of liquids is also a way to modify the dynamics of a liquid and the properties of a glass; it corresponds to a large number of situations encountered in nature. Another phase diagram $T - d$ (d defining pore size) can be defined with a non-trivial pore size dependence of the glass transition, which is also strongly affected by surface interactions.

Une catégorie importante de matériaux vitrifiables est de nature organique ; elle comprend les liquides moléculaires, les polymères, les solutions, les protéines qui peuvent être vitrifiés par refroidissement du liquide dans des conditions standard ou après des traitements thermiques spéciaux. La gamme d’applications est vaste, allant de la science des matériaux aux sciences de la vie et plus récemment à l’électronique. Afin de les distinguer des autres systèmes décrits dans ce numéro, certaines propriétés spécifiques telles que le domaine de température de transition vitreuse ( $T_{g}$ ), leur capacité à former un verre et quelques règles empiriques pour localiser $T_{g}$ sont présentées. Cependant la propriété la plus remarquable de ces liquides, qui les distinguent des autres classes de matériaux, est la rapidité avec laquelle leur viscosité ou leur temps de relaxation structural augmente à l’approche de $T_{g}$ . Afin de caractériser ce comportement et de classer les liquides, C.A. Angell a introduit le concept de fragilité il y a près de 40 ans. Il a proposé de nommer les liquides comme fragiles ou forts dans un diagramme d’Arrhenius en fonction de $T_{g} / T$ (les plus forts n’ont jamais été observés pour les verres organiques, sauf l’eau sous des conditions particulières). La valeur de $T_{g}$ et la fragilité d’un liquide donné peuvent être modifiées en appliquant une pression, c’est-à-dire en changeant la densité. On peut alors explorer les propriétés du liquide surfondu et surcomprimé, et celles du verre dans un diagramme de phase $P - T$ . La ligne de transition vitreuse correspond à une ligne isochrone, c’est-à-dire une ligne à temps de relaxation constant avec différents couples densité-température. Nous avons observé que toutes les données peuvent être placées sur des courbes maîtresses qui ne dépendent que d’une seule énergie d’activation effective, $E_{\infty} (ρ)$ dépendante de la densité et de l’espèce et indépendante de la température. Un indice de fragilité isochore est défini comme une propriété intrinsèque d’un liquide donné qui peut aider à rationaliser toutes les corrélations entre les propriétés des verres en dessous de $T_{g}$ et le ralentissement visqueux juste au-dessus de $T_{g}$ . Le confinement géométrique des liquides est également un moyen de modifier la dynamique d’un liquide et les propriétés d’un verre ; il correspond à un grand nombre de situations rencontrées dans la nature. Un autre diagramme de phase $T - d$ (d= diamètre des pores) peut être défini avec une dépendance non triviale de la transition vitreuse par rapport à la taille des pores, fortement affectée par les interactions de surface.

Received: 2022-09-26
Revised: 2023-01-27
Accepted: 2023-02-21
Online First: 2023-08-03
Published online: 2024-04-26

DOI: 10.5802/crphys.148

Keywords: molecular liquids and glasses, polymers, fragility, density scaling, correlations
Mots-clés : liquides moléculaires et verres, polymères, fragilité, loi d’échelle en densité, corrélations entre dynamiques rapide et lente

Author's affiliations:

Christiane Alba-Simionesco ¹

¹ Laboratoire Léon Brillouin, Université Paris-Saclay, CEA, CNRS, 91191, Gif-sur-Yvette, France

License:

CC-BY 4.0

Copyrights: The authors retain unrestricted copyrights and publishing rights

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Christiane Alba-Simionesco. Organic Glass-Forming Liquids and the Concept of Fragility. Comptes Rendus. Physique, From everyday glass to disordered solids, Volume 24 (2023) no. S1, pp. 177-198. doi : 10.5802/crphys.148. https://comptes-rendus.academie-sciences.fr/physique/articles/10.5802/crphys.148/

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