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Title: Theory for Glassy Behavior of Supercooled Liquid Mixtures

Abstract

Here, we introduce a model for glassy dynamics in supercooled liquid mixtures. Given the relaxation behavior of individual supercooled liquids, the model predicts the relaxation times of their mixtures as temperature is decreased. The model is based on dynamical facilitation theory for glassy dynamics, which provides a physical basis for relaxation and vitrification of a supercooled liquid. This is in contrast to empirical linear interpolations such as the Gordon-Taylor equation typically used to predict glass transition temperatures of liquid mixtures. To understand the behavior of supercooled liquid mixtures we consider a multicomponent variant of the kinetically constrained East model in which components have a different energy scale and can also diffuse when locally mobile regions, i.e., excitations, are present. Using a variational approach we confirm an effective single component model with a single effective energy scale that best approximates a mixture. When scaled by this single effective energy, we show that experimental relaxation times of many liquid mixtures all collapse onto the "parabolic law" predicted by dynamical facilitation theory. The model can be used to predict transport properties and glass transition temperatures of mixtures of glassy materials, with implications in atmospheric chemistry, biology, and pharmaceuticals.

Authors:
 [1];  [2];  [3]
  1. Univ. of California, Berkeley, CA (United States)
  2. Univ. of Nottingham (United Kingdom)
  3. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1572838
Alternate Identifier(s):
OSTI ID: 1560716
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 123; Journal Issue: 10; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Katira, Shachi, Garrahan, Juan P., and Mandadapu, Kranthi K. Theory for Glassy Behavior of Supercooled Liquid Mixtures. United States: N. p., 2019. Web. doi:10.1103/physrevlett.123.100602.
Katira, Shachi, Garrahan, Juan P., & Mandadapu, Kranthi K. Theory for Glassy Behavior of Supercooled Liquid Mixtures. United States. https://doi.org/10.1103/physrevlett.123.100602
Katira, Shachi, Garrahan, Juan P., and Mandadapu, Kranthi K. Thu . "Theory for Glassy Behavior of Supercooled Liquid Mixtures". United States. https://doi.org/10.1103/physrevlett.123.100602. https://www.osti.gov/servlets/purl/1572838.
@article{osti_1572838,
title = {Theory for Glassy Behavior of Supercooled Liquid Mixtures},
author = {Katira, Shachi and Garrahan, Juan P. and Mandadapu, Kranthi K.},
abstractNote = {Here, we introduce a model for glassy dynamics in supercooled liquid mixtures. Given the relaxation behavior of individual supercooled liquids, the model predicts the relaxation times of their mixtures as temperature is decreased. The model is based on dynamical facilitation theory for glassy dynamics, which provides a physical basis for relaxation and vitrification of a supercooled liquid. This is in contrast to empirical linear interpolations such as the Gordon-Taylor equation typically used to predict glass transition temperatures of liquid mixtures. To understand the behavior of supercooled liquid mixtures we consider a multicomponent variant of the kinetically constrained East model in which components have a different energy scale and can also diffuse when locally mobile regions, i.e., excitations, are present. Using a variational approach we confirm an effective single component model with a single effective energy scale that best approximates a mixture. When scaled by this single effective energy, we show that experimental relaxation times of many liquid mixtures all collapse onto the "parabolic law" predicted by dynamical facilitation theory. The model can be used to predict transport properties and glass transition temperatures of mixtures of glassy materials, with implications in atmospheric chemistry, biology, and pharmaceuticals.},
doi = {10.1103/physrevlett.123.100602},
journal = {Physical Review Letters},
number = 10,
volume = 123,
place = {United States},
year = {Thu Sep 05 00:00:00 EDT 2019},
month = {Thu Sep 05 00:00:00 EDT 2019}
}

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Works referenced in this record:

Relaxation Dynamics in Glycerol−Water Mixtures:  I. Glycerol-Rich Mixtures
journal, March 2005

  • Puzenko, Alexander; Hayashi, Yoshihito; Ryabov, Yaroslav E.
  • The Journal of Physical Chemistry B, Vol. 109, Issue 12
  • DOI: 10.1021/jp0445122

Relaxation processes in supercooled liquids
journal, March 1992


Mixing Effects for the Structural Relaxation in Binary Hard-Sphere Liquids
journal, August 2003


Corresponding States of Structural Glass Formers
journal, April 2009

  • Elmatad, Yael S.; Chandler, David; Garrahan, Juan P.
  • The Journal of Physical Chemistry B, Vol. 113, Issue 16
  • DOI: 10.1021/jp810362g

Amorphous pharmaceutical solids: preparation, characterization and stabilization
journal, May 2001


Ideal copolymers and the second-order transitions of synthetic rubbers. i. non-crystalline copolymers
journal, September 1952


Dynamics on the Way to Forming Glass: Bubbles in Space-Time
journal, March 2010


Structural Relaxation Dynamics in Binary Glass-Forming Molecular Liquids with Ideal and Complex Mixing Behavior
journal, March 2010

  • Wang, Li-Min; Tian, Yongjun; Liu, Riping
  • The Journal of Physical Chemistry B, Vol. 114, Issue 10
  • DOI: 10.1021/jp912223j

Equilibrium Sampling of Hard Spheres up to the Jamming Density and Beyond
journal, June 2016


Microscopic Theory of Heterogeneity and Nonexponential Relaxations in Supercooled Liquids
journal, June 2001


Evolution of organic aerosol mass spectra upon heating: implications for OA phase and partitioning behavior
journal, January 2011


An amorphous solid state of biogenic secondary organic aerosol particles
journal, October 2010

  • Virtanen, Annele; Joutsensaari, Jorma; Koop, Thomas
  • Nature, Vol. 467, Issue 7317
  • DOI: 10.1038/nature09455

Characteristics and Significance of the Amorphous State in Pharmaceutical Systems
journal, January 1997

  • Hancock, Bruno C.; Zografi, George
  • Journal of Pharmaceutical Sciences, Vol. 86, Issue 1
  • DOI: 10.1021/js9601896

The role of Vitrification in Anhydrobiosis
journal, October 1998


Geometrical Explanation and Scaling of Dynamical Heterogeneities in Glass Forming Systems
journal, July 2002


Binary Glass-Forming Materials:  Mixtures of Sorbitol and Glycerol
journal, July 2004

  • Duvvuri, Kalyan; Richert, Ranko
  • The Journal of Physical Chemistry B, Vol. 108, Issue 29
  • DOI: 10.1021/jp031366b

A hierarchically constrained kinetic Ising model
journal, February 1991

  • J�ckle, J.; Eisinger, S.
  • Zeitschrift f�r Physik B Condensed Matter, Vol. 84, Issue 1
  • DOI: 10.1007/BF01453764

Time scale separation in the low temperature East model: rigorous results
journal, April 2013

  • Chleboun, P.; Faggionato, A.; Martinelli, F.
  • Journal of Statistical Mechanics: Theory and Experiment, Vol. 2013, Issue 04
  • DOI: 10.1088/1742-5468/2013/04/L04001

Beta Relaxation versus High Frequency Wing in the Dielectric Spectra of a Binary Molecular Glass Former
journal, June 2004


Thermodynamics of glasses: a first principles computation
journal, January 1999


Solvation in Space-time: Pretransition Effects in Trajectory Space
journal, June 2018


Implication of glass transition for the drying and stability of dried foods
journal, May 1999


Glass transition temperatures for simple molecular liquids and their binary solutions
journal, November 1978

  • Angell, C. A.; Sare, J. M.; Sare, E. J.
  • The Journal of Physical Chemistry, Vol. 82, Issue 24
  • DOI: 10.1021/j100513a016

Glassy dynamics in the asymmetrically constrained kinetic Ising chain
journal, September 2003


Fast simulation of facilitated spin models
journal, December 2005

  • Ashton, Douglas J.; Hedges, Lester O.; Garrahan, Juan P.
  • Journal of Statistical Mechanics: Theory and Experiment, Vol. 2005, Issue 12
  • DOI: 10.1088/1742-5468/2005/12/P12010

Glassy dynamics of kinetically constrained models
journal, June 2003


Models of Hierarchically Constrained Dynamics for Glassy Relaxation
journal, September 1984


Coarse-grained microscopic model of glass formers
journal, August 2003

  • Garrahan, J. P.; Chandler, D.
  • Proceedings of the National Academy of Sciences, Vol. 100, Issue 17
  • DOI: 10.1073/pnas.1233719100

Ideal Mixing Behavior of the Debye Process in Supercooled Monohydroxy Alcohols
journal, May 2005

  • Wang, Li-Min; Richert, Ranko
  • The Journal of Physical Chemistry B, Vol. 109, Issue 18
  • DOI: 10.1021/jp050342x

Glassy Time-Scale Divergence and Anomalous Coarsening in a Kinetically Constrained Spin Chain
journal, October 1999


Excitations Are Localized and Relaxation Is Hierarchical in Glass-Forming Liquids
journal, November 2011


On the Temperature Dependence of Cooperative Relaxation Properties in Glass‐Forming Liquids
journal, July 1965

  • Adam, Gerold; Gibbs, Julian H.
  • The Journal of Chemical Physics, Vol. 43, Issue 1
  • DOI: 10.1063/1.1696442

Morphology of mixed primary and secondary organic particles and the adsorption of spectator organic gases during aerosol formation
journal, March 2010

  • Vaden, T. D.; Song, C.; Zaveri, R. A.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 15
  • DOI: 10.1073/pnas.0911206107

Equilibrium and Non-Equilibrium Type β-Relaxations:  d -Sorbitol versus o -Terphenyl
journal, May 1999

  • Wagner, Hermann; Richert, Ranko
  • The Journal of Physical Chemistry B, Vol. 103, Issue 20
  • DOI: 10.1021/jp9838947

Relaxation in glassforming liquids and amorphous solids
journal, September 2000

  • Angell, C. A.; Ngai, K. L.; McKenna, G. B.
  • Journal of Applied Physics, Vol. 88, Issue 6
  • DOI: 10.1063/1.1286035

Calorimetric glass transition explained by hierarchical dynamic facilitation
journal, March 2013

  • Keys, A. S.; Garrahan, J. P.; Chandler, D.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 12
  • DOI: 10.1073/pnas.1302665110

Glass transition and phase state of organic compounds: dependency on molecular properties and implications for secondary organic aerosols in the atmosphere
journal, January 2011

  • Koop, Thomas; Bookhold, Johannes; Shiraiwa, Manabu
  • Physical Chemistry Chemical Physics, Vol. 13, Issue 43
  • DOI: 10.1039/c1cp22617g

Supercooled Liquids and Glasses
journal, January 1996

  • Ediger, M. D.; Angell, C. A.; Nagel, Sidney R.
  • The Journal of Physical Chemistry, Vol. 100, Issue 31
  • DOI: 10.1021/jp953538d

Phase relations and vitrification in saccharide-water solutions and the trehalose anomaly
journal, April 1989

  • Green, J. L.; Angell, C. A.
  • The Journal of Physical Chemistry, Vol. 93, Issue 8
  • DOI: 10.1021/j100345a006

Morphology of mixed primary and secondary organic particles and the adsorption of spectator organic gases during aerosol formation
journal, March 2010

  • Vaden, T. D.; Song, C.; Zaveri, R. A.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 15
  • DOI: 10.1073/pnas.0911206107

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