Multiple dynamic regimes in concentrated microgel systems

Abstract

We investigate dynamical heterogeneities in the collective relaxation of a concentrated microgel system, for which the packing fraction can be conveniently varied by changing the temperature. The packing fraction dependent mechanical properties are characterised by a fluid-solid transition, where the system properties switch from a viscous to an elastic low-frequency behaviour. Approaching this transition from below, we find that the range of spatial correlations in the dynamics increases. Beyond this transition, the spatial correlation range reaches a maximum, extending over the entire observable system size of approximately 5 mm. Increasing the packing fraction even further leads to a second transition, which is characterised by the development of large zones of lower and higher dynamical activity that are well separated from each other; the range of correlation decreases at this point. This striking non-monotonic dependence of the spatial correlation length on volume fraction is reminiscent of the behaviour recently observed at the jamming/rigidity transition in granular systems (Lechenault et al. 2008). We identify this second transition as the transition to 'squeezed' states, where the constituents of the system start to exert direct contact forces on each other, such that the dynamics becomes increasingly determined by imbalanced stresses. Evidence of this transition is also found in the frequency dependence of the storage and loss moduli, which become increasingly coupled as direct friction between the particles starts to contribute to the dissipative losses within the system. To our knowledge, our data provide the first observation of a qualitative change in dynamical heterogeneity as the dynamics switch from purely thermally-driven to stress-driven.

19 pages, 8 figures. Latest version corrects errors in the indication of the concentration of microgel systems and the equation for the temperature dependence of the particle radius

References in corpus (5)

• Probing the equilibrium dynamics of colloidal hard spheres above the mode-coupling glass transition
• Time Resolved Correlation measurements of temporally heterogeneous dynamics
• Critical scaling and heterogeneous superdiffusion across the jamming/rigidity transition of a granular glass
• Resolving long-range spatial correlations in jammed colloidal systems using photon correlation imaging
• Unexpected drop of dynamical heterogeneities in colloidal suspensions approaching the jamming transition

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• Superdiffusive, heterogeneous, and collective particle motion near the jamming transition in athermal disordered materials
• Equilibrium properties of charged microgels: a Poisson-Boltzmann-Flory approach
• Density-Temperature-Softness Scaling of the Dynamics of Glass-forming Soft-sphere Liquids
• Centrifugal compression of soft particle packings - theory and experiment
• Scaling of the glassy dynamics of soft repulsive particles: a mode-coupling approach
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• Dynamical heterogeneity in soft particle suspensions under shear
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• Overcharging and reentrant condensation of thermoresponsive ionic microgels
• Nucleation and growth of micellar polycrystals under time-dependent volume fraction conditions
• Structural relaxation, dynamical arrest and aging in soft-sphere liquids