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Register a new userStrain Heterogeneity in Sheared Colloids Revealed by Neutron Scattering
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Recent computational and theoretical studies have shown that the deformation of colloidal suspensions under a steady shear is highly heterogeneous at the particle level and demonstrate a critical influence on the macroscopic deformation behavior. Despite its relevance to a wide variety of industrial applications of colloidal suspensions, scattering studies focusing on addressing the heterogeneity of the non-equilibrium colloidal structure are scarce thus far. Here, we report the first experimental result using small-angle neutron scattering. From the evolution of strain heterogeneity, we conclude that the shear-induced deformation transforms from nearly affine behavior at low shear rates, to plastic rearrangements when the shear rate is high.
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The microscopic deformation mechanism of charged colloidal glasses with extended-range interactions under shear is investigated by in-situ small-angle neutron scattering, and a dynamically correlated region (DCR) is identified. This short-lived region provides the resistance to the configurational rearrangement imposed by the external deformation, as evidenced by the evolution of the size of DCR in the shear thinning regime and the quantitative agreement between the local stress sustained by DCR and the macroscopic stress from rheological measurements at low and mediate shear rates. This finding suggests that DCR is an important quantity for microscopically addressing the flow and deformation behavior of strongly interacting colloids.
The flow of colloidal suspensions is ubiquitous in nature and industry. Colloidal suspensions exhibit a wide range of rheological behavior, which should be closely related to the microscopic structure of the systems. With in-situ small-angle neutron scattering complemented by rheological measurements, we investigated the deformation behavior of a charge-stabilized colloidal glass at particle level undergoing steady shear. A short-lived, localized elastic response at particle level, termed as transient elasticity zone (TEZ), was identified from the neutron spectra. The existence of the TEZ is a signature of the dynamical heterogeneity: The body of fluids under shear behaves like an elastic solid within the spatial range of TEZ but like fluid outside the TEZ. The size of TEZ shrinks as the shear rate increases in the shear thinning region, which shows that the shear thinning is accompanied by a diminishing dynamical heterogeneity. More interestingly, the TEZ is found to be the structural unit that provides the resistance to the imposed shear, as evidenced by the quantitative agreement between the local elastic stress sustained by TEZ and the macroscopic stress from rheological measurements at low and moderate shear rates. Besides the charged-stabilized colloidal suspension, a hard-sphere colloidal suspension at the same volume fraction and shear rates was also measured. The result highlights the key role of the electrostatic interparticle repulsion in promoting the local elasticity. Our findings provide an understanding on the nonlinear rheology of interacting colloidal glasses from a micro-mechanical view.
Application of shear flow to charge-stabilized aqueous colloidal suspensions is ubiquitous in industrial applications and as a means to achieve controlled field-induced assembly of nanoparticles. Yet, applying shear flow to a charge-stabilized colloidal suspension, which is initially monodisperse and in quasi-equilibrium leads to non-trivial clustering phenomena (and sometimes to a gelation transition), dominated by the complex interplay between DLVO interactions and shear flow. The quantitative understanding of these strongly nonequilibrium phenomena is still far from being complete. By taking advantage of a recent shear-induced aggregation rate theory developed in our group, we present here a systematic numerical study, based on the governing master kinetic equation (population-balance) for the shear-induced clustering and breakup of colloids exposed to shear flow. In the presence of sufficiently stable particles, the clustering kinetics is characterized by an initial very slow growth, controlled by repulsion. During this regime, particles are slowly aggregating to form clusters, the reactivity of which increases along with their size growth. When their size reaches a critical threshold, a very rapid, explosive-like growth follows, where shear forces are able to overcome the energy barrier between particles. This stage terminates when a dynamic balance between shear-induced aggregation and cluster breakage is reached. It is also observed that these systems are characterized by a cluster mass distribution that for a long time presents a well-defined bimodality. The model predictions are quantitatively in excellent agreement with available experimental data, showing how the theoretical picture is able to quantitatively account for the underlying nonequilibrum physics.
Using small angle neutron scattering, we conducted a detailed structural study of poly(3-alkylthiophenes) dispersed in deuterated dicholorbenzene. The focus was placed on addressing the influence of spatial arrangement of constituent atoms of side chain on backbone conformation. We demonstrate that by impeding the {pi}- {pi} interactions, the branch point in side chain promotes torsional motion between backbone units and results in greater chain flexibility. Our findings highlight the key role of topological isomerism in determining the molecular rigidity and are relevant to the current debate about the condition necessary for optimizing the electronic properties of conducting polymers via side chain engineering.
Interface localization-delocalization transitions (ILDT) occur in two-phase fluids confined in a slit with competing preferences of the walls for the two fluid phases. At low temperatures the interface between the two phases is localized at one of the walls. Upon increasing temperature it unbinds. Although intensively studied theoretically and computationally, such transitions have not yet been observed experimentally due to severe challenges in resolving fine details of the fluid structure. Here, using mean field theory and Monte Carlo simulations of the Ising model, we propose to detect these ILDT by using colloids. We show that the finite-size and fluctuation induced force acting on a colloid confined in such a system experiences a vivid change if, upon lowering the temperature, the interface localizes at one of the walls. This change can serve as a more easily accessible experimental indicator of the transition.
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