The concentrated noncolloidal suspensions show complex rheological behavior, which is related to the existence of contact stress. However, determining the contact stress in time-varying flow like oscillatory shear is challenging. Herein, we propose a contact stress decomposition method to decompose the total stress directly into contact stress and hydrodynamic stress in large amplitude oscillatory shear (LAOS). The results of hydrodynamic stress and contact stress are consistent with those determined by the shear reversal experiment. The contact stress decomposition also explains the failure of the Cox–Merz rule in noncolloidal suspensions because the particle contacts exist in steady shear but are absent in small amplitude oscillatory shear. The intracycle and intercycle of contact stress are further analyzed through the general geometric average method. The intracycle behaviors exhibit strain hardening, strain softening, and shear thickening. The intercycle behaviors show bifurcations in stress-strain and stress-strain rate relations, where the transition strains at different concentrations define the state boundaries between the discrete particle contacts, the growing of particle contacts, and the saturated contacts. We also established a phenomenological constitutive model using a structural parameter to describe the shear effect on the buildup and breakdown of particle contacts. The contact stress of noncolloidal suspensions with wide ranges of particle concentrations and strain amplitudes under LAOS can be well described by the model.
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See supplementary material online for Fig. S1: the particle size and quantity distribution; Fig. S2: the relative error between the two methods in determining
and
; Fig. S3: the stress-strain rate curves of 44.1% suspension; Fig. S4: the ratio of maximum contact stress versus strain amplitude; Fig. S5:
versus strain amplitude; Fig. S6:
versus the apparent critical strain
of strain hardening; Fig. S7: representative stress versus time curves for shear cessation experiment; Fig. S8: comparison of the SR experiment and the SD method under
; Fig. S9: stress-strain rate relation of 44.1% suspension under different strain amplitudes; Fig. S10: comparisons on
and
between this work and Lemaire et al. [55]; Fig. S11: stress-strain, stress-strain rate curve at strain amplitude 0.25, and the moduli versus frequency at small strain amplitude; Fig. S12: the comparison of the contact stress obtained by the stress decomposition method and SP model; Fig. S13:
versus
and
versus
; Fig. S14: A11 versus strain, A11 versus strain rate, N1 and contact stress versus strain, N1 and contact stress versus strain rate under strain amplitude 2.5; Fig. S15: ratio between N1 and shear stress and maximum of N1/σ versus particle concentration.
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