Fragile-to-Strong Crossover, growing length scales, and dynamic heterogeneity in Wigner Glasses

TL;DR

This study uses simulations of Wigner glasses to demonstrate a continuous fragile-to-strong transition driven by particle softness, confirming RFOT theory's predictions about growing correlation lengths and dynamic heterogeneity in glass formation.

Contribution

It shows that tuning particle softness in Wigner glasses induces a fragile-to-strong transition, validating RFOT theory's universal applicability to glassy dynamics.

Findings

Continuous fragile-to-strong transition observed

Correlation length grows as predicted by RFOT

Dynamic heterogeneity increases with correlation length

Abstract

Colloidal particles, which are ubiquitous, have become ideal testing grounds for the structural glass transition (SGT) theories. In these systems glassy behavior is manifested 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. By performing Brownian dynamics simulations for a binary mixture of micron-sized charged colloidal suspensions, known to form Wigner glasses, we show that by tuning the softness of the potential, achievable by changing the monovalent salt concentration, there is a continuous transition between fragile to strong behavior. Remarkably, this is found in a system where the well characterized 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, $\xi\sim (\phi_K/\phi - 1)^{-\nu}$ with $\nu = 2/3$ where $\phi_K$, the analogue 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. The broad range of fragility observed in Wigner glasses is used to draw analogies with molecular glasses. The large variations in the fragility is 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, implying that the physics describing the SGT is universal.