Field-induced gelation, yield stress, and fragility of an electro-rheological suspension

Electro-rheological suspensions (ERS) are known to undergo liquid-to-solid transition under the application of an electric field. Long-range interaction between neighboring particles results in sample-spanning particulate structures which behave as soft solids. Here, we studied the rheological expression of this field-induced transition which has many similarities with chemical gelation. This similarity shows in mechanical spectroscopy on a suspension of monodisperse silica in PDMS as model ERS. Upon application of the electric field, dynamic moduli G', G grow by orders of magnitude and evolve in a pattern which is otherwise typical for gelation of network polymers (random chemical or physical gelation). At the gel point. the slow dynamics is governed by power-law relaxation behavior (frequency-independent tan delta). A low field strength is sufficient to reach the gel point and, correspondingly, the percolating particle structure at the eel point is still very fragile. It can be broken by the imposition of low stress. For inducing a finite yield stress, the field strength needs to be increased further until the long-range electrostatic interaction generates string-like particle alignments which become clearly visible under the optical microscope. The onset of fragile connectivity was defined experimentally by the tan delta method. The ERS was probed dynamically at low frequencies where the transition is most pronounced, and also in steady shear where the rate of structure formation equals the rate of internal breaking.