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Tuning the solubility of fuzzy polymer microgels by external triggers, such as temperature or pH, provides a unique mechanism for controlling the porosity and size of colloidal particles on the nanoscale. As a consequence, these smart microgel particles are being considered for applications ranging from viscosity modifiers and sensing to drug delivery and as models for the glass and the jamming transition. Despite their widespread use, little is known about how these soft particles adapt their shape and size under strong mechanical compression. We use a combination of precise labeling protocols and two-color superresolution microscopy to unravel the behavior of tracer microgels inside densely packed soft solids. We find that interpenetration and shape deformation are dominant until, in the highly overpacked state, this mechanism saturates and the only remaining way to further densify the system is by isotropic compression.

Thermosensitive microgels are widely studied hybrid systems combining properties of polymers and colloidal particles in a unique way. Due to their complex morphology, their interactions and packing, and consequentially the viscoelasticity of suspensions made from microgels, are still not fully understood, in particular under dense packing conditions. Here we study the frequency-dependent linear viscoelastic properties of dense suspensions of micron sized soft particles in conjunction with an analysis of the local particle structure and morphology based on superresolution microscopy. By identifying the dominating mechanisms that control the elastic and dissipative response, we can explain the rheology of these widely studied soft particle assemblies from the onset of elasticity deep into the overpacked regime. Interestingly, our results suggest that the friction between the microgels is reduced due to lubrification mediated by the polymer brush-like corona before the onset of interpenetration.

Tuning the solubility of fuzzy polymer microgels by external triggers, such as temperature or pH, provides a unique mechanism for controlling the porosity and size of colloidal particles on the nanoscale. As a consequence, these smart microgel particles are being considered for applications ranging from viscosity modifiers and sensing to drug delivery and as models for the glass and the jamming transition. Despite their widespread use, little is known about how these soft particles adapt their shape and size under strong mechanical compression. We use a combination of precise labeling protocols and two-color superresolution microscopy to unravel the behavior of tracer microgels inside densely packed soft solids. We find that interpenetration and shape deformation are dominant until, in the highly overpacked state, this mechanism saturates and the only remaining way to further densify the system is by isotropic compression.