Rheology of Dense Suspensions under Shear Rotation.

Dense non-Brownian suspensions exhibit a spectacular and abrupt drop in viscosity under change of shear direction, as revealed by shear inversions (reversals) or orthogonal superposition. Here, we introduce an experimental setup to systematically explore their response to shear rotations, where one suddenly rotates the principal axes of shear by an angle θ, and measure the shear stresses with a biaxial force sensor. Our measurements confirm the genericness of the transient decrease of the resistance to shear under unsteady conditions.

Effect of Particle Specific Surface Area on the Rheology of Non-Brownian Silica Suspensions.

Industrial formulations very often involve particles with a broad range of surface characteristics and size distributions. Particle surface asperities (roughness) and porosity increase particle specific surface area and significantly alter suspension rheology, which can be detrimental to the quality of the end product. We examine the rheological properties of two types of non-Brownian, commercial precipitated silicas, with varying specific surface area, namely PS52 and PS226, suspended in a non-aqueous solvent, glycerol, and compare them against those of glass sphere suspensions (GS2) with a similar size distribution.

Microfluidic liquid cell chamber for scanning probe microscopy measurement application.

In this paper, we present a universal microfluidic liquid chamber device platform for atomic force microscopy (AFM), which enables to fabricate the uniform lipid bilayer on the hydrophilic surface using the solvent-assisted lipid bilayer formation method. Using this device enables us to acquire the various properties of delicate soft matter, including morphological data, and mechanical property measurements, using high-resolution AFM systems. The proposed technology is expected to provide an understanding of complicated biological materials.

A Numerical Study on the Effect of Particle Surface Coverage on the Quartz Crystal Microbalance Response.

The quartz crystal microbalance (QCM) is a surface-sensitive measurement technique to characterize adsorption processes at solid-fluid interfaces. While QCM measurements are routinely applied to study homogeneous thin films, characterizing heterogeneous films of adsorbed particles remains challenging because QCM is sensitive to not only the mass of adsorbed particles but also to that of hydrodynamically coupled fluid. To extract information about adsorbed particles, it is necessary to model these hydrodynamic effects, however, current QCM models are restricted to the limit of either a very low surface coverage or to the extrapolated limit of saturation coverage.

Effect of Glucose on the Mobility of Membrane-Adhering Liposomes.

Enclosed lipid bilayer structures, referred to as liposomes or lipid vesicles, have a wide range of biological functions, such as cellular signaling and membrane trafficking. The efficiency of cellular uptake of liposomes, a key step in many of these functions, is strongly dependent on the contact area between a liposome and a cell membrane, which is governed by the adhesion force w, the membrane bending energy κ, and the osmotic pressure Δp. Herein, we investigate the relationship between these forces and the physicochemical properties of the solvent, namely, the presence of glucose (a nonionic osmolyte).

Quartz Crystal Microbalance Model for Quantitatively Probing the Deformation of Adsorbed Particles at Low Surface Coverage.

Characterizing the deformation of nanoscale, soft-matter particulates at solid-liquid interfaces is a demanding task, and there are limited experimental options to perform quantitative measurements in a nonperturbative manner. Previous attempts, based on the quartz crystal microbalance (QCM) technique, focused on the high surface coverage regime and modeled the adsorbed particles as a homogeneous film, while not considering the coupling between particles and surrounding fluid and hence resulting in an underestimation of the known particle height. In this work, we develop a model for the hydrodynamic coupling between adsorbed particles and surrounding fluid in the limit of a low surface coverage, which can be used to extract shape information from QCM measurement data.

A model derived from hydrodynamic simulations for extracting the size of spherical particles from the quartz crystal microbalance.

One challenging aspect of quartz crystal microbalance (QCM) measurements is the characterization of adsorbed particles as the change in resonance frequency (Δf) is proportional not only to the inertia of the adsorbed layer but also to that of the hydrodynamically coupled fluid. Herein, by solving numerically the Navier-Stokes equations, we scrutinize Δf for sparsely deposited, rigid spherical particles that are firmly attached to an oscillating surface. The analysis is shown to be applicable to adsorbed, small unilamellar vesicles (SUVs) of controlled size under experimental conditions in which adhesion-induced vesicle deformation is negligible.

Probing Membrane Viscosity and Interleaflet Friction of Supported Lipid Bilayers by Tracking Electrostatically Adsorbed, Nano-Sized Vesicles.

Particle tracking is used to measure the diffusional motion of nanosized (≈100 nm), lipid vesicles that are electrostatically adsorbed onto a solid supported lipid bilayer. It is found that the motion of membrane-adhering vesicles is Brownian and depends inversely on the vesicle size, but is insensitive to the vesicle surface charge. The measured diffusivity agrees well with the Evans-Sackmann model for the diffusion of inclusions in supported, fluidic membranes.

Hydrodynamic Propulsion of Liposomes Electrostatically Attracted to a Lipid Membrane Reveals Size-Dependent Conformational Changes.

The efficiency of lipid nanoparticle uptake across cellular membranes is strongly dependent on the very first interaction step. Detailed understanding of this step is in part hampered by the large heterogeneity in the physicochemical properties of lipid nanoparticles, such as liposomes, making conventional ensemble-averaging methods too blunt to address details of this complex process. Here, we contribute a means to explore whether individual liposomes become deformed upon binding to fluid cell-membrane mimics.

A phenomenological model of the solvent-assisted lipid bilayer formation method.

The recently introduced solvent-assisted lipid bilayer (SALB) formation method allows one to efficiently fabricate planar, lipid bilayers on solid supports and can be used for various applications. It involves the introduction of an aqueous buffer into a mixture of lipid and alcohol, which is incubated on a solid support. The associated phase changes in the ternary bulk system are accompanied by the formation of a lipid bilayer at the solid-liquid interface.

Size-dependent, stochastic nature of lipid exchange between nano-vesicles and model membranes.

The interaction of nanoscale lipid vesicles with cell membranes is of fundamental importance for the design and development of vesicular drug delivery systems. Here, we introduce a novel approach to study vesicle-membrane interactions whereby we are able to probe the influence of nanoscale membrane properties on the dynamic adsorption, exchange, and detachment of vesicles. Using total internal reflection fluorescence (TIRF) microscopy, we monitor these processes in real-time upon the electrostatically tuned attachment of individual, sub-100 nm vesicles to a supported lipid bilayer.

Brownian Dynamics of Electrostatically Adhering Small Vesicles to a Membrane Surface Induces Domains and Probes Viscosity.

Using single-particle tracking, we investigate the interaction of small unilamellar vesicles (SUVs) that are electrostatically tethered to the freestanding membrane of a giant unilamellar vesicle (GUV). We find that the surface mobility of the GUV-riding SUVs is Brownian, insensitive to the bulk viscosity, vesicle size, and vesicle fluidity but strongly altered by the viscosity of the underlying membrane. Analyzing the diffusional behavior of SUVs within the Saffman-Delbrück model for the dynamics of membrane inclusions supports the notion that the mobility of the small vesicles is coupled to that of dynamically induced lipid clusters within the target GUV membrane.

Spatiotemporal dynamics of solvent-assisted lipid bilayer formation.

The solvent-assisted lipid bilayer (SALB) method offers a general strategy to fabricate supported lipid bilayers on solid surfaces. In this method, lipids dissolved in alcohol are deposited on the target substrate in parallel with their aggregation during exchange with aqueous buffer solution which promotes spontaneous bilayer formation. Herein, a combination of experimental and theoretical approaches is employed in order to understand the key aspects of the SALB formation process.