Glass Transition and Yielding of Ultrasoft Charged Spherical Micelles

Colloids are widely used as model systems to study the glass transition, with much research focused on hard or soft neutral colloids and their mixtures. However, the glass transition of soft-charged spherical colloids and its dynamic effects remain underexplored. This study assesses the glass transition of polymeric multiarm charged soft colloids using shear rheology, coarse-grained molecular dynamics (MD) simulations, and X-ray scattering. Strong particle–particle correlations, driven by electrostatic interarm repulsion, inhibit Newtonian behavior in the dilute regime. The liquid-to-glass transition occurs at just 0.25 wt %, marked by weak caging and minimal interdigitation of arms, as evidenced by particle contact analysis in MD simulations and the strong frequency dependence of the dynamic moduli. Particle shells interdigitate only well within the glassy regime, leading to a nearly frequency-independent rheological response. The weak volume fraction dependence of the yield stress sets these charged systems among the softest colloids reported in the literature.