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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 Lab. (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. doi: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. doi:10.1103/physrevlett.123.100602.
@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 = {2019},
month = {9}
}

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