Literature DB >> 23576746

Why glass elasticity affects the thermodynamics and fragility of supercooled liquids.

Le Yan1, Gustavo Düring, Matthieu Wyart.   

Abstract

Supercooled liquids are characterized by their fragility: The slowing down of the dynamics under cooling is more sudden and the jump of specific heat at the glass transition is generally larger in fragile liquids than in strong ones. Despite the importance of this quantity in classifying liquids, explaining what aspects of the microscopic structure controls fragility remains a challenge. Surprisingly, experiments indicate that the linear elasticity of the glass--a purely local property of the free energy landscape--is a good predictor of fragility. In particular, materials presenting a large excess of soft elastic modes, the so-called boson peak, are strong. This is also the case for network liquids near the rigidity percolation, known to affect elasticity. Here we introduce a model of the glass transition based on the assumption that particles can organize locally into distinct configurations that are coupled spatially via elasticity. The model captures the mentioned observations connecting elasticity and fragility. We find that materials presenting an abundance of soft elastic modes have little elastic frustration: Energy is insensitive to most directions in phase space, leading to a small jump of specific heat. In this framework strong liquids turn out to lie the closest to a critical point associated with a rigidity or jamming transition, and their thermodynamic properties are related to the problem of number partitioning and to Hopfield nets in the limit of small memory.

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Year:  2013        PMID: 23576746      PMCID: PMC3631624          DOI: 10.1073/pnas.1300534110

Source DB:  PubMed          Journal:  Proc Natl Acad Sci U S A        ISSN: 0027-8424            Impact factor:   11.205


  25 in total

1.  A thermodynamic connection to the fragility of glass-forming liquids.

Authors:  L M Martinez; C A Angell
Journal:  Nature       Date:  2001-04-05       Impact factor: 49.962

2.  Role of the interaction matrix in mean-field spin glass models.

Authors:  R Cherrier; D S Dean; A Lefèvre
Journal:  Phys Rev E Stat Nonlin Soft Matter Phys       Date:  2003-04-21

3.  Correlations of the nonexponentiality and state dependence of mechanical relaxations with bond connectivity in Ge-As-Se supercooled liquids.

Authors: 
Journal:  Phys Rev B Condens Matter       Date:  1992-05-01

4.  On the Adam-Gibbs-Kirkpatrick-Thirumalai-Wolynes scenario for the viscosity increase in glasses.

Authors:  Jean-Philippe Bouchaud; Giulio Biroli
Journal:  J Chem Phys       Date:  2004-10-15       Impact factor: 3.488

5.  Fragility of Ge-As-Se glass-forming liquids in relation to rigidity percolation, and the Kauzmann paradox.

Authors: 
Journal:  Phys Rev Lett       Date:  1990-03-26       Impact factor: 9.161

6.  Correlations between vibrational entropy and dynamics in liquids.

Authors:  Matthieu Wyart
Journal:  Phys Rev Lett       Date:  2010-03-01       Impact factor: 9.161

7.  Correlation of fragility of supercooled liquids with elastic properties of glasses.

Authors:  V N Novikov; Y Ding; A P Sokolov
Journal:  Phys Rev E Stat Nonlin Soft Matter Phys       Date:  2005-06-06

8.  Elasticity of floppy and stiff random networks.

Authors:  M Wyart; H Liang; A Kabla; L Mahadevan
Journal:  Phys Rev Lett       Date:  2008-11-19       Impact factor: 9.161

9.  Effective-medium theory of percolation on central-force elastic networks. II. Further results.

Authors: 
Journal:  Phys Rev B Condens Matter       Date:  1985-06-01

10.  Neural networks and physical systems with emergent collective computational abilities.

Authors:  J J Hopfield
Journal:  Proc Natl Acad Sci U S A       Date:  1982-04       Impact factor: 11.205

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  6 in total

1.  The kinetic fragility of liquids as manifestation of the elastic softening.

Authors:  F Puosi; D Leporini
Journal:  Eur Phys J E Soft Matter       Date:  2015-08-13       Impact factor: 1.890

2.  Quantitative relations between cooperative motion, emergent elasticity, and free volume in model glass-forming polymer materials.

Authors:  Beatriz A Pazmiño Betancourt; Paul Z Hanakata; Francis W Starr; Jack F Douglas
Journal:  Proc Natl Acad Sci U S A       Date:  2015-02-23       Impact factor: 11.205

3.  Understanding, predicting, and tuning the fragility of vitrimeric polymers.

Authors:  Simone Ciarella; Rutger A Biezemans; Liesbeth M C Janssen
Journal:  Proc Natl Acad Sci U S A       Date:  2019-11-25       Impact factor: 11.205

4.  Quasilocalized states of self stress in packing-derived networks.

Authors:  Edan Lerner
Journal:  Eur Phys J E Soft Matter       Date:  2018-08-21       Impact factor: 1.890

Review 5.  Temperature Dependence of Structural Relaxation in Glass-Forming Liquids and Polymers.

Authors:  Vladimir N Novikov; Alexei P Sokolov
Journal:  Entropy (Basel)       Date:  2022-08-10       Impact factor: 2.738

6.  Entropy favors heterogeneous structures of networks near the rigidity threshold.

Authors:  Le Yan
Journal:  Nat Commun       Date:  2018-04-10       Impact factor: 14.919

  6 in total

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