PubMed Health⌕ Search

Biomedical subjects

Eric M Furst

Publications and source records attributed to Eric M Furst.

10 recordsLinked to original sources

Colloid dynamics in semiflexible polymer solutions.

We investigate the dynamics of monodisperse colloidal polystyrene particles suspended in solutions of the semiflexible polymer filamentous actin, over a range of filament lengths that either exceed or are substantially less than the particle radius. The filament length is controlled by the capping protein gelsolin, and particle surface chemistries that minimize the adsorption of filaments are used. The particle dynamics are measured on short time scales using diffusing wave spectroscopy. A sharp transition in the initial particle diffusivity marks the expected shift from a dilute to a tightly entangled polymer network as the filament average length increases. In both the dilute and entangled regimes, the measured particle dynamics are compared with the theories of rodlike and semiflexible polymer solution rheology using the generalized Stokes-Einstein relationship. In the dilute limit, the particle dynamics are in good agreement with theory. However, in the tightly entangled regime, the particle response is consistent with polymer depleted near the surfaces of the particles. The magnitude of the depletion layer thickness depends strongly on particle size and weakly on filament length. This behavior is in agreement with nonlocal entropic repulsions and the loss of conformational entropy associated with rodlike molecules near impenetrable particles. These results illustrate the use of microrheology as a method to investigate local structure and dynamics in colloid-polymer solutions.

Journal Article↗

Formation and evolution of sediment layers in an aggregating colloidal suspension.

The coupled aggregation and sedimentation of colloidal particles with short-range attractions are investigated. Nonadsorbing polymer is used to induce depletion interactions between the hard-sphere particles. Gravitational forces, caused by a density mismatch between the particles and the suspending fluid, result in the sedimentation of particles and aggregates, as well as the compaction and rearrangement of the final sediment layer. At low polymer concentrations CP, or low initial volume fractions phio, clusters formed during the period of fast sedimentation are small, and the structure of the final sediment is dense. Conversely, at high CP, or high phio, large clusters form during sedimentation, and the resulting sediment structure is significantly less dense, with large void volumes. The size of the presediment aggregates depends on CP and phio with a functional form that resembles other thermally activated barrier hopping processes in colloidal systems, such as the delayed sedimentation of colloidal gels. Finally, when the particles are weakly attractive, gravitational stresses are found to induce compaction of the sediment over long periods of time. However, sediments composed of particles that are strongly attractive resist rearrangements and compaction, even when the sediment layers have a relatively large amount of free volume.

Journal Article↗

Manipulation of hydrogel assembly and growth factor delivery via the use of peptide-polysaccharide interactions.

The design of materials in which assembly, mechanical response, and biological properties are controlled by protein-polysaccharide interactions could provide materials that mimic the biological environment and find use in the delivery of growth factors. In the investigations reported here, a heparin-binding, coiled-coil peptide, PF4 ZIP, was employed to mediate the assembly of heparinized polymers. The heparin-binding affinity of this peptide was compared with that of other heparin-binding peptides (HBP) via heparin-sepharose chromatography and surface plasmon resonance (SPR) experiments. Results from these experiments indicate that PF4 ZIP demonstrates a higher heparin-binding affinity and heparin association rate when compared to the heparin-binding domains of antithrombin III (ATIII) and heparin-interacting protein (HIP). Viscoelastic hydrogels were formed upon the association of PF4 ZIP-functionalized star poly(ethylene glycol) (PEG-PF4 ZIP) with low-molecular-weight heparin-functionalized star PEG (PEG-LMWH). The viscoelastic properties of the hydrogels can be altered via variations in the ratio of LMWH to PF4 ZIP. bFGF release from these gels have also been investigated. Comparison of the bFGF release profiles with the hydrogel erosion profiles indicates that bFGF delivery from this class of hydrogels is mainly an erosion-controlled process and the rates of bFGF release can be modulated via choice of HBP or via variations in the mechanical properties of the hydrogels. Manipulation of hydrogel physical properties and erosion profiles will provide novel materials for controlled growth factor delivery and other biomedical applications.

Algorithms↗

Colloidal aggregate micromechanics in the presence of divalent ions.

Colloidal gels exhibit rheological properties, such as a yield stress and elasticity, which arise from the manner in which stress is transmitted through the microstructure. Insight into the mechanisms of stress transmission is critical in developing a full understanding of the mechanics of these materials. Paramount to this is a thorough knowledge of the interparticle interactions. In this work, we use optical trapping to study interactions between poly(methyl methacrylate) (PMMA) particles in adhesive contact by measuring the bending elasticity of directly assembled colloidal aggregates under various physicochemical conditions. The simplified geometry of the aggregate enables us determine the single-bond rigidity, which can then be related to the work of adhesion, W(SL), through the Johnson-Kendall-Roberts (JKR) theory of adhesion. We find that W(SL) is independent of ionic strength in flocculating monovalent salt solutions. However, more complex behavior is observed for divalent salts. Using zeta-potential measurements, we show that divalent cations adsorb to the particle surface. This results in the formation of ionic bridges between particles in adhesive contact. A model of the aggregate micromechanics that considers the divalent ion contribution to the surface energy provides a direct link between the interfacial properties of the particles, nanoscale contact interactions between particles, and the bulk gel modulus.

Journal Article↗

Synthesis of monodisperse fluorescent core-shell silica particles using a modified Stober method for imaging individual particles in dense colloidal suspensions.

Core-shell silica particles, with a diameter of 1.5 mum, containing a dye fluorescein isothiocyanate (FITC), are synthesized by the hydrolysis and condensation of tetraethylorthosilicate (TEOS). Sodium dodecyl sulfate (SDS) is added to synthesize fluorescent core particles with the diameter of approximately 1 mum. In the addition of SDS, the surface charge reduced by counterions (Na+) of the surfactant leads to a higher degree of aggregation of the primary particles and the formation of larger secondary particles. The particle growth kinetics confirms the aggregation growth model for the synthesis of monodisperse silica particles, and also shows the dependence of final particle size on colloidal stability resulting from the addition of SDS. Light and X-ray scattering data reveal that the final particles have compactly packed structures with smooth surfaces. The seeded growth technique is then used to form a silica shell layer on the fluorescent core. The added amount of water and NH4OH has significant effects on shell formation. Finally, the final core-shell silica particles are modified by chemisorption of octadecanol at the surface to be dispersed in organic solvents. Octadecyl-coated silica particles are sterically stabilized in silica index-matching solvents such as chloroform and hexadecane to directly image separate particles using confocal microscopy. In chloroform, the organophilic silica particles disperse well, whereas in hexadecane they form a volume-filling gel structure at room temperature.

Journal Article↗

Elasticity and critical bending moment of model colloidal aggregates.

The bending mechanics of singly bonded colloidal aggregates are measured using laser tweezers. We find that the colloidal bonds are capable of supporting significant torques, providing a direct measurement of the tangential interactions between particles. A critical bending moment marks the limit of linear bending elasticity, past which small-scale rearrangements occur. These mechanical properties underlie the rheology and dynamics of colloidal gels formed by diffusion-limited cluster aggregation, and give critical insight into the contact interactions between Brownian particles.

Journal Article↗

Probe surface chemistry dependence and local polymer network structure in F-actin microrheology.

We investigate the dependence of F-actin microrheology on probe surface chemistry using diffusing wave spectroscopy. Polystyrene probe particles exhibit subdiffusive mean-squared displacements, where Deltar(2)(t) approximately t(0.77)(+/-)(0.03) consistent with previous experiments and theory. However, polystyrene probes preadsorbed with bovine serum albumin (BSA) interact weakly with the surrounding polymer network and exhibit a scaling exponent similar to pure diffusion Deltar(2)(t) approximately t, which decreases as particle size and actin concentration increases. Using models of particle diffusion in locally heterogeneous viscoelastic microenvironments, we find that the microrheological response of BSA-treated particles is consistent with the formation of a polymer-depleted shell surrounding the probes. The shell thickness scales with particle size but not polymer concentration. These results suggest that the depletion is caused by exclusion or orientation of actin filaments near probes due to their long length and rigidity.

Actins↗

Directed assembly and rupture mechanics of colloidal aggregates.

The macroscopic rheological behavior of colloidal gels arises from the micromechanical properties of the gel backbone, which are governed by nanoscale particle interactions. These colloidal interactions have been commonly understood in terms of the Derjaguin-Landau-Verwey-Overbeek (DLVO) theory. Recent work has shown, however, that nonidealities, such as surface roughness and charge nonuniformity, may cause the particle interactions to significantly deviate from DLVO predictions at near-contact separations. Here we present novel techniques for directing the assembly of colloidal aggregates that mimic the gel backbone, based on optical micromanipulation of multiple particles using laser tweezers. This also provides an in situ method for measuring near-contact interactions via single-bond rupture forces. We find that PMMA particles aggregated in the presence of nonorganic salts exhibit interparticle bond strengths more than 10 times greater than those predicted by DLVO theory. However, good agreement is found with DLVO predictions when the anionic surfactant sodium dodecyl sulfate (SDS) is used as the flocculant.

Journal Article↗

Motor-driven dynamics in actin-myosin networks.

The effect of myosin motor protein activity on the filamentous actin (F-actin) rheological response is studied using diffusing wave spectroscopy. Under conditions of saturating motor activity, we find an enhancement of longitudinal filament fluctuations corresponding to a scaling of the viscoelastic shear modulus G(d)(omega) approximately omega(7/8). As the adenosine tri-phosphate reservoir sustaining motor activity is depleted, we find an abrupt transient to a passive, "rigor state" and a return to dissipation dominated by transverse filament modes. Single-filament measurements of the apparent persistence length support the notion that motor activity leads to an increase in the effective temperature for tangential motion.

Actins↗

Rheological characterization of polysaccharide-poly(ethylene glycol) star copolymer hydrogels.

Binding interactions between low molecular weight heparin (LMWH) and heparin-binding peptides (HBP) have been applied as a strategy for the assembly of hydrogels that are capable of sequestering growth factors and delivering them in a controlled manner. In this work, the assembly of four-arm star poly(ethylene glycol) (PEG)-LMWH conjugate with PEG-HBP conjugates has been investigated. The interactions between LMWH and the heparin-binding regions of antithrombin III (ATIII) or the heparin interacting protein (HIP) have been characterized via heparin affinity chromatography and surface plasmon resonance (SPR); results indicate that the two peptides have slightly different affinities for heparin and LMWH, and bind LMWH with micromolar affinity. Solutions of the PEG-LMWH and of mixtures of the PEG-LMWH and PEG-HBP were characterized via both bulk rheology and laser tweezer microrheology. Interestingly, solutions of PEG-LMWH (2.5 wt % in PBS) form hydrogels in the absence of PEG-ATIII or PEG-HIP, with storage moduli, determined via bulk rheological measurements, in excess of the loss moduli over frequencies of 0.1-100 Hz. The addition of PEG-ATIII or PEG-HIP increases the moduli in direct proportion to the number of cross-links introduced. Characterization of the hydrogels via microrheology shows the gel microstructure is composed of polymer-rich fibrillar structures surrounded by polymer-depleted buffer. Potential applications of these hydrogels are discussed.

Amino Acid Sequence↗