A three-dimensional lattice gas model for amphiphilic fluid dynamics

We describe a three-dimensional hydrodynamic lattice-gas model of amphiphilic fluids. This model of the non-equilibrium properties of oil-water-surfactant systems, which is a non-trivial extension of an earlier two-dimensional realisation due to Boghosian, Coveney and Emerton [Boghosian, Coveney, and Emerton 1996, Proc. Roy. Soc. A 452, 1221-1250], can be studied effectively only when it is implemented using high-performance computing and visualisation techniques. We describe essential aspects of the model's theoretical basis and computer implementation, and report on the phenomenological properties of the model which confirm that it correctly captures binary oil-water and surfactant-water behaviour, as well as the complex phase behaviour of ternary amphiphilic fluids.Comment: 34 pages, 13 figures, high resolution figures available on reques

Spatiotemporal dynamics of multiple shear-banding events for viscoelastic micellar fluids in cone-plate shearing flows

We characterize the transient response of semi-dilute wormlike micellar solutions under an imposed steady shear flow in a cone-plate geometry. By combining conventional rheometry with 2-D Particle Image Velocimetry (PIV), we can simultaneously correlate the temporal stress response with time-resolved velocimetric measurements. By imposing a well defined shear history protocol, consisting of a stepped shear flow sweep, we explore both the linear and nonlinear responses of two surfactant solutions: cetylpiridinium chloride (CPyCl) and sodium salicylate (NaSal) mixtures at concentrations of [66:40] mM and [100:60] mM, respectively. The transient stress signal of the more dilute solution relaxes to its equilibrium value very fast and the corresponding velocity profiles remain linear, even in the strongly shear-thinning regime. The more concentrated solution also exhibits linear velocity profiles at small shear rates. At large enough shear rates, typically larger than the inverse of the relaxation time of the fluid, the flow field reorganizes giving rise to strongly shear-banded velocity profiles. These are composed of an odd number of shear bands with low-shear-rate bands adjacent to both gap boundaries. In the non-linear regime long transients (much longer than the relaxation time of the fluid) are observed in the transient stress response before the fluid reaches a final, fully-developed state. The temporal evolution in the shear stress can be correlated with the spatiotemporal dynamics of the multiple shear-banded structure measured using RheoPIV. In particular our experiments show the onset of elastic instabilities in the flow which are characterized by the presence of multiple shear bands that evolve and rearrange in time resulting in a slow increase in the average torque acting on the rotating fixture

Structure, Rheology and Optical Properties of Plasmonic Fluids

Fluids with tunable optical and rheological properties are of fundamental and practical interest. They can be easily processed to manufacture thin films and interfaces for applications such as molecular detection and light trapping in photovoltaics. Cationic surfactants such as cetyl-trimethylammonium bromide have the ability to self assemble with metallic nanoparticles to form a corona or a double-layer vesicular structure. These structures upon further interaction with wormlike micelle fragments are hypothesized to form micelle-nanoparticle elastic networks. In this dissertation, solution phase self-assembly is utilized to uniformly distribute various metallic nanoparticles to produce stable multicomponent plasmonic fluids with remarkable color uniformity. The optical properties of the fluids can be robustly tuned by varying the species, concentration, size and/or shape of the nanoparticles. Multicomponent plasmonic fluids capable of broadband absorption of visible light are produced via the self-assembly route. Small angle X-ray scattering and rheological studies suggest that the nanoparticles are incorporated into the wormlike micelle network to form a more compact double network. These fluids exhibit rich rheological behavior depending on the nanoparticle concentration and the salt to surfactant molar ratio. Specifically, non-monotonic dependence of zero shear viscosity on nanoparticle concentration, rheopexy, shear thickening, shear banding and shear thinning are observed. The fluids exhibit enhanced viscoelasticity upon the addition of more nanoparticles. The mechanical, rheological and optical properties of plasmonic fluids greatly depend upon the temperature due to the structural changes of the micellar solutions. The application of plasmonic fluids to efficient light trapping in photovoltaic cells, plasmon-enhanced microalgal growth and optofluidic devices have been designed and demonstrated in this dissertation

Probing shear-banding transitions of the VCM model for entangled wormlike micellar solutions using large amplitude oscillatory shear (LAOS) deformations

We explore the use of large amplitude oscillatory shear (LAOS) deformation to probe the dynamics of shear-banding in soft entangled materials, primarily wormlike micellar solutions which are prone to breakage and disentanglement under strong deformations. The state of stress in these complex fluids is described by a class of viscoelastic constitutive models which capture the key linear and nonlinear rheological features of wormlike micellar solutions, including the breakage and reforming of an entangled network. At a frequency-dependent critical strain, the imposed deformation field localizes to form a shear band, with a phase response that depends on the frequency and amplitude of the forcing. The different material responses are compactly represented in the form of Lissajous (phase plane) orbits and a corresponding strain-rate and frequency-dependent Pipkin diagram. Comparisons between the full network model predictions and those of a simpler, limiting case are presented.National Science Foundation (U.S.) (NSF DMS-0807395)National Science Foundation (U.S.) (NSF DMS-0807330

Phase Separation of Rigid-Rod Suspensions in Shear Flow

We analyze the behavior of a suspension of rigid rod-like particles in shear flow using a modified version of the Doi model, and construct diagrams for phase coexistence under conditions of constant imposed stress and constant imposed strain rate, among paranematic, flow-aligning nematic, and log-rolling nematic states. We calculate the effective constitutive relations that would be measured through the regime of phase separation into shear bands. We calculate phase coexistence by examining the stability of interfacial steady states and find a wide range of possible ``phase'' behaviors.Comment: 23 pages 19 figures, revised version to be published in Physical Review