Dynamic
viscoelasticity and dynamic birefringence of a microgel
system were investigated around the liquid–solid transition
concentration to clarify the molecular origin of the viscoelastic
response of the microgel system. The complex modulus showed viscoelastic
liquid-like behavior at concentrations, c, below
a threshold c
jamming for random close
packing of the microgels, whereas viscoelastic solid-like behavior
at c > c
jamming. The
imaginary part of the complex strain-optical coefficient changed its
sign with increasing angular frequency ω in a liquid-like regime,
suggesting that the stress and birefringence involved three relaxation
mechanisms. Utilizing the stress-optical rule, SOR, for each relaxation
process, the complex shear modulus at c < c
jamming was separated into the orientational
stress of network strands in temporary contacted microgels, deformation
of particle, and the redistribution process, from high frequencies
in this order. On the other hand, in a solid-like regime at c > c
jamming, the ordinary
SOR
held well with a single stress-optical coefficient, C, implying that only one stress origin is dominant, which can be
attributed to the orientational stress of densely packed microgels
in permanent contact. The strain-optical coefficients evaluated using
the Onuki–Doi theory reproduced the measurements qualitatively
and supported these assignments.