Literature DB >> 18927234

Facilitation, complexity growth, mode coupling, and activated dynamics in supercooled liquids.

Sarika Maitra Bhattacharyya1, Biman Bagchi, Peter G Wolynes.   

Abstract

In low-temperature-supercooled liquids, below the ideal mode-coupling theory transition temperature, hopping and continuous diffusion are seen to coexist. Here, we present a theory that shows explicitly the interplay between the two processes and shows that activated hopping facilitates continuous diffusion in the otherwise frozen liquid. Several universal features arise from nonlinear interactions between the continuous diffusive dynamics described here by the mode coupling theory (MCT)] and the activated hopping (described here by the random first-order transition theory). We apply the theory to a specific system, Salol, to show that the theory correctly predicts the temperature dependence of the nonexponential stretching parameter, beta, and the primary alpha relaxation timescale, tau. The study explains why, even below the mean field ergodic to nonergodic transition, the dynamics is well described by MCT. The nonlinear coupling between the two dynamical processes modifies the relaxation behavior of the structural relaxation from what would be predicted by a theory with a complete static Gaussian barrier distribution in a manner that may be described as a facilitation effect. Furthermore, the theory correctly predicts the observed variation of the stretching exponent beta with the fragility parameter, D. These two predictions also allow the complexity growth to be predicted, in good agreement with the results of Capaccioli et al. [Capaccioli S, Ruocco G, Zamponi F (2008) J Phys Chem B 112:10652-10658].

Mesh:

Year:  2008        PMID: 18927234      PMCID: PMC2570993          DOI: 10.1073/pnas.0808375105

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


  14 in total

1.  Fragilities of liquids predicted from the random first order transition theory of glasses.

Authors:  X Xia; P G Wolynes
Journal:  Proc Natl Acad Sci U S A       Date:  2000-03-28       Impact factor: 11.205

2.  Microscopic theory of heterogeneity and nonexponential relaxations in supercooled liquids.

Authors:  X Xia; P G Wolynes
Journal:  Phys Rev Lett       Date:  2001-06-11       Impact factor: 9.161

3.  Anisotropic local stress and particle hopping in a deeply supercooled liquid.

Authors:  Sarika Bhattacharyya; Biman Bagchi
Journal:  Phys Rev Lett       Date:  2002-06-24       Impact factor: 9.161

4.  Brillouin scattering in salol: Determining Tc of the mode coupling theory.

Authors: 
Journal:  Phys Rev Lett       Date:  1992-12-21       Impact factor: 9.161

5.  Direct experimental evidence of a growing length scale accompanying the glass transition.

Authors:  L Berthier; G Biroli; J-P Bouchaud; L Cipelletti; D El Masri; D L'Hôte; F Ladieu; M Pierno
Journal:  Science       Date:  2005-12-16       Impact factor: 47.728

6.  Crossover behavior and multistep relaxation in a schematic model of the cut-off glass transition.

Authors:  M J Greenall; M E Cates
Journal:  Phys Rev E Stat Nonlin Soft Matter Phys       Date:  2007-05-15

7.  Spatial correlations in the dynamics of glassforming liquids: experimental determination of their temperature dependence.

Authors:  C Dalle-Ferrier; C Thibierge; C Alba-Simionesco; L Berthier; G Biroli; J-P Bouchaud; F Ladieu; D L'Hôte; G Tarjus
Journal:  Phys Rev E Stat Nonlin Soft Matter Phys       Date:  2007-10-29

8.  Intermolecular forces and the glass transition.

Authors:  Randall W Hall; Peter G Wolynes
Journal:  J Phys Chem B       Date:  2007-11-09       Impact factor: 2.991

9.  Light-scattering investigation of alpha and beta relaxation near the liquid-glass transition of the molecular glass Salol.

Authors: 
Journal:  Phys Rev A       Date:  1992-09-15       Impact factor: 3.140

10.  Trap models and slow dynamics in supercooled liquids.

Authors:  R Aldrin Denny; David R Reichman; Jean-Philippe Bouchaud
Journal:  Phys Rev Lett       Date:  2003-01-17       Impact factor: 9.161

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  11 in total

1.  Positron annihilation response and broadband dielectric spectroscopy: salol.

Authors:  J Bartoš; M Iskrová; M Köhler; R Wehn; O Sauša; P Lunkenheimer; J Krištiak; A Loidl
Journal:  Eur Phys J E Soft Matter       Date:  2011-09-26       Impact factor: 1.890

2.  Dynamical facilitation governs glassy dynamics in suspensions of colloidal ellipsoids.

Authors:  Chandan K Mishra; K Hima Nagamanasa; Rajesh Ganapathy; A K Sood; Shreyas Gokhale
Journal:  Proc Natl Acad Sci U S A       Date:  2014-10-13       Impact factor: 11.205

3.  On the surface of glasses.

Authors:  Jacob D Stevenson; Peter G Wolynes
Journal:  J Chem Phys       Date:  2008-12-21       Impact factor: 3.488

4.  Growing length and time scales in glass-forming liquids.

Authors:  Smarajit Karmakar; Chandan Dasgupta; Srikanth Sastry
Journal:  Proc Natl Acad Sci U S A       Date:  2009-02-20       Impact factor: 11.205

5.  Spatiotemporal structures in aging and rejuvenating glasses.

Authors:  Peter G Wolynes
Journal:  Proc Natl Acad Sci U S A       Date:  2009-02-02       Impact factor: 11.205

6.  Dynamical theory of shear bands in structural glasses.

Authors:  Apiwat Wisitsorasak; Peter G Wolynes
Journal:  Proc Natl Acad Sci U S A       Date:  2017-01-20       Impact factor: 11.205

7.  Continuous-time random-walk approach to supercooled liquids: Self-part of the van Hove function and related quantities.

Authors:  J Helfferich; J Brisch; H Meyer; O Benzerara; F Ziebert; J Farago; J Baschnagel
Journal:  Eur Phys J E Soft Matter       Date:  2018-06-01       Impact factor: 1.890

8.  On the strength of glasses.

Authors:  Apiwat Wisitsorasak; Peter G Wolynes
Journal:  Proc Natl Acad Sci U S A       Date:  2012-09-17       Impact factor: 11.205

9.  Soft Vibrational Modes Predict Breaking Events during Force-Induced Protein Unfolding.

Authors:  Mona Habibi; Steven S Plotkin; Jörg Rottler
Journal:  Biophys J       Date:  2018-02-06       Impact factor: 4.033

10.  A universal origin for secondary relaxations in supercooled liquids and structural glasses.

Authors:  Jacob D Stevenson; Peter G Wolynes
Journal:  Nat Phys       Date:  2009-01-01       Impact factor: 20.034

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