Phase behavior of colloid-polymer mixtures with unary or binary depletants

Submicron particles suspended in solutions containing surfactants, polymers, micelles, or other species are widely used in materials shaping and forming processes, including three-dimensional printing and nanocomposite processing, and in technical applications as paints, coatings, inks, and drilling muds. These applications require control over suspension rheology and microstructure, which are affected by interactions between the different constituents. Practically, constituents of high dispersity in size or molecular weight are inexpensive and hence widely used; fundamentally, the effects of size dispersity on suspension properties remain poorly understood when the particles exhibit attractive as well as repulsive interparticle interactions. As simple models of practical suspensions we formulate mixtures of submicron poly(methyl methacrylate) (PMMA) particles suspended in solutions of non adsorbing polystyrene polymers, which generate a controlled entropic depletion attraction between the particles. Here, I will discuss studies in which we investigate the effect of polymer dispersity on the phase behavior, microstructure, and rheology of colloid-polymer mixtures. We added unary or binary mixtures of polystyrene as the depletant to suspensions of charged PMMA particles. The structure and dynamics of the particles were compared over three sets of samples with various mixtures of two different polystyrenes whose size varied by an order of magnitude. The structure and dynamics were nearly independent of depletant dispersity if the polymer concentration was represented as a sum of normalized concentrations of each species. Near the transition region between a fluid of clusters and an interconnected gel at intermediate volume fractions, partitioning of polymers in a binary mixture into colloid-rich and polymer-rich phase leads to a slightly different gelation pathway. Hence this work suggests that polymers of high dispersity, which are more affordable than uniformly distributed polymers, can be used for applications requiring certain final structures if all polymers in the distribution are small compared to the particles and if the desired phase behavior is far from non-equilibrium boundaries. It also suggests the ability to tune the final polymer concentration by mixing polymers of different sizes to control particle phase behavior in solution. Please click Additional Files below to see the full abstract

Tunable Assembly of Gold Nanorods in Polymer Solutions to Generate Controlled Nanostructured Materials

Gold nanorods grafted with short chain polymers are assembled into controlled open structures using polymer-induced depletion interactions and structurally characterized using small angle x-ray scattering. When the nanorod diameter is smaller than the radius of gyration of the depletant polymer, the depletion interaction depends solely on the correlation length of the polymer solution and not directly on the polymer molecular weight. As the polymer concentration increases, the stronger depletion interactions increasingly compress the grafted chains and push the gold nanorods closer together. By contrast, other structural characteristics such as the number of nearest neighbors and fractal dimension exhibit a non-monotonic dependence on polymer concentration. These parameters are maximal at intermediate concentrations, which are attributed to a crossover from reaction-limited to diffusion-limited aggregation. The control over structural properties of anisotropic nanoscale building blocks demonstrated here will be beneficial to designing and producing materials \emph{in situ} with specific direction-dependent nanoscale properties and provides a crucial route for advances in additive manufacturing

Bacteria Use Type IV Pili to Walk Upright and Detach from Surfaces

1. Department of Bioengineering, California Nano Systems Institute,University of California, Los Angeles, CA 90024, USA. 2. Department of Chemical and Biomolecular Engineering, University of Houston, Houston, TX 77204, USA. 3. Department of Materials Science and Engineering, University of Illinois, Urbana-Champaign, IL 61801, USA. 4. Department of Civil Engineering and Geological Sciences, University of Notre Dame, Notre Dame, IN 46556, USA.Bacterial biofilms are structured multicellular communities involved in a broad range of infections. Knowing how free-swimming bacteria adapt their motility mechanisms near surfaces is crucial for understanding the transition between planktonic and biofilm phenotypes. By translating microscopy movies into searchable databases of bacterial behavior, we identified fundamental type IV pili–driven mechanisms for Pseudomonas aeruginosa surface motility involved in distinct foraging strategies. Bacteria stood upright and “walked” with trajectories optimized for two-dimensional surface exploration. Vertical orientation facilitated surface detachment and could influence biofilm morphology.Center for Nonlinear Dynamic

Increasing Binding Efficiency via Reporter Shape and Flux in a Viral Nanoparticle Lateral-Flow Assay

To identify factors controlling the performance of reporter particles in a sensitive lateral-flow assay (LFA), we investigated the effect of the flux and shape of filamentous bacteriophage (phage) on the performance of phage LFAs. Phage of three different lengths and diameters were modified with biotin and AlexaFluor 555 as binding and read-out elements, respectively. The binding efficiencies of the functionalized phage were tested in a fibrous glass LFA membrane modified with avidin. The total binding rate, quantified using real-time particle counting and particle image velocimetry, decreased monotonically with the average bulk flux of phage through the membrane. At the pore scale, more phage bound in regions with faster local flow, confirming that both average and local flux increased binding. The number of bound phage increased with the aspect ratio of the phage and scaled with the phage surface area, consistent with a binding interaction controlled by the number of recognition elements on the surface. Together, these results indicate that increasing the likelihood that recognition elements on the surface of phage encounter the fibers enhances the assay binding efficiency and suggests one origin for the improved performance of nonspherical phage reporters

Orientational binding modes of reporters in a viral-nanoparticle lateral flow assay

Using microscopy and image analysis, we characterize binding of filamentous viral nanoparticles to a fibrous affinity matrix as models for reporter capture in a lateral flow assay (LFA). M13 bacteriophage (M13) displaying an in vivo-biotinylated peptide (AviTag) genetically fused to the M13 tail protein p3 are functionalized with fluorescent labels. We functionalize glass fiber LFA membranes with antibodies to M13, which primarily capture M13 on the major p8 coat proteins, or with avidin, which captures M13 at the biotin-functionalized tail, and compare orientational modes of reporter capture for the side- versus tip-binding recognition interactions. The number of captured M13 is greater for side-binding than for tip-binding, as expected from the number of recognition groups. Whereas two-thirds of side-bound M13 captured by an anti-M13 antibody bind immediately after colliding with the membrane, tip-bound M13 prominently exhibit three additional orientational modes that require M13 to reorient to enable binding. These results are consistent with the idea that the elongated M13 shape couples with the complex flow field in an open and disordered fibrous LFA membrane to enhance capture

Aptamer-Phage Reporters for Ultrasensitive Lateral Flow Assays

We introduce the modification of bacteriophage particles with aptamers for use as bioanalytical reporters, and demonstrate the use of these particles in ultrasensitive lateral flow assays. M13 phage displaying an in vivo biotinylatable peptide (AviTag) genetically fused to the phage tail protein pIII were used as reporter particle scaffolds, with biotinylated aptamers attached via avidin朾iotin linkages, and horseradish peroxidase (HRP) reporter enzymes covalently attached to the pVIII coat protein. These modified viral nanoparticles were used in immunochromatographic sandwich assays for the direct detection of IgE and of the penicillin-binding protein from Staphylococcus aureus (PBP2a). We also developed an additional lateral flow assay for IgE, in which the analyte is sandwiched between immobilized anti-IgE antibodies and aptamer-bearing reporter phage modified with HRP. The limit of detection of this LFA was 0.13 ng/mL IgE, ?100 times lower than those of previously reported IgE assays

Flotation Immunoassay: Masking the Signal from Free Reporters in Sandwich Immunoassays

In this work, we demonstrate that signal-masking reagents together with appropriate capture antibody carriers can eliminate the washing steps in sandwich immunoassays. A flotation immunoassay (FI) platform was developed with horseradish peroxidase chemiluminescence as the reporter system, the dye Brilliant Blue FCF as the signal-masking reagent, and buoyant silica micro-bubbles as the capture antibody carriers. Only reporters captured on micro-bubbles float above the dye and become visible in an analyte-dependent manner. These FIs are capable of detecting proteins down to attomole levels and as few as 106 virus particles. This signal-masking strategy represents a novel approach to simple, sensitive and quantitative immunoassays in both laboratory and point-of-care settings