Theory for Glassy Behavior of Supercooled Liquid Mixtures

Katira, Shachi; Garrahan, Juan P.; Mandadapu, Kranthi K.

doi:10.1103/physrevlett.123.100602

Theory for Glassy Behavior of Supercooled Liquid Mixtures

Journal Article · Thu Sep 05 04:00:00 EDT 2019 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.123.100602· OSTI ID:1572838

Katira, Shachi ^[1]; Garrahan, Juan P. ^[2]; Mandadapu, Kranthi K. ^[3]

Univ. of California, Berkeley, CA (United States)
Univ. of Nottingham (United Kingdom)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1572838

Alternate ID(s):: OSTI ID: 1560716

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 10 Vol. 123; ISSN 0031-9007; ISSN PRLTAO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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