Fragile-to-strong crossover, growing length scales, and dynamic heterogeneity in Wigner glasses

Hyun Woo Cho, Mauro L. Mugnai, T. R. Kirkpatrick, and D. Thirumalai
Phys. Rev. E 101, 032605 – Published 17 March 2020

Abstract

Colloidal particles, which are ubiquitous, have become ideal testing grounds for the structural glass transition theories. In these systems glassy behavior arises as the density of the particles is increased. Thus, soft colloidal particles with varying degree of softness capture diverse glass-forming properties, observed normally in molecular glasses. Brownian dynamics simulations for a binary mixture of micron-sized charged colloidal suspensions show that tuning the softness of the interaction potential, achievable by changing the monovalent salt concentration results in a continuous transition from fragile to strong behavior. Remarkably, this is found in a system where the well characterized interaction potential between the colloidal particles is isotropic. We also show that the predictions of the random first-order transition (RFOT) theory quantitatively describes the universal features such as the growing correlation length, ξϕKϕ1ν with ν=23 where ϕK, the analog of the Kauzmann temperature, depends on the salt concentration. As anticipated by the RFOT predictions, we establish a causal relationship between the growing correlation length and a steep increase in the relaxation time and dynamic heterogeneity as the system is compressed. The broad range of fragility observed in Wigner glasses is used to draw analogies with molecular and polymer glasses. The large variations in the fragility are normally found only when the temperature dependence of the viscosity is examined for a large class of diverse glass-forming materials. In sharp contrast, this is vividly illustrated in a single system that can be experimentally probed. Our work also shows that the RFOT predictions are accurate in describing the dynamics over the entire density range, regardless of the fragility of the glasses.

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  • Received 17 September 2019
  • Accepted 26 February 2020

DOI:https://doi.org/10.1103/PhysRevE.101.032605

©2020 American Physical Society

Physics Subject Headings (PhySH)

Polymers & Soft Matter

Authors & Affiliations

Hyun Woo Cho1, Mauro L. Mugnai1, T. R. Kirkpatrick2, and D. Thirumalai1

  • 1Department of Chemistry, University of Texas at Austin, Austin, Texas 78712, USA
  • 2Institute for Physical Science and Technology, University of Maryland, College Park, Maryland 20742, USA

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Vol. 101, Iss. 3 — March 2020

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