Novel measurements of the spatiotemporal microstructure of a continuous shear thickening colloidal suspension under shear cessation and reversal using small angle neutron scattering in a 1–2 shear cell are presented for moderate to high Péclet numbers. In the shear cessation experiments from high Péclet shear flow, two-step relaxation mechanism is found. Particles first readily diffuse on a characteristic timescale of single particle Brownian motion, followed by slower relaxation dynamics on a timescale of short-time self-diffusion when caging effects start dominating. In the shear reversal experiment, the unchanged scattering intensity and the quick flip in anisotropic structure around the shear thickened state suggest the persistence of hydroclusters without transitioning through the equilibrium structure, at least in a time resolution of 0.01 s. Access to the time evolution of microstructure provides valuable insights into the spatiotemporal details of interparticle interactions governing colloidal suspension rheology, such as Brownian, hydrodynamic, and nanotribological forces.
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