Aidan T. Brown

Ionic effects in self-propelled Pt-coated Janus swimmers

Colloidal particles partially coated with platinum and dispersed in H2O2 solution are often used as model self-propelled colloids. Most current data suggest that neutral self-diffusiophoresis propels these particles. However, several studies have shown strong ionic effects in this and related systems, such as a reduction of propulsion speed by salt. We investigate these ionic effects in Pt-coated polystyrene colloids, and find here that the direction of propulsion can be reversed by addition of an ionic surfactant, and that although adding pH neutral salts reduces the propulsion speed, adding the strong base NaOH has little effect. We use these data, as well as measured reaction rates, to argue against propulsion by either neutral or ionic self-diffusiophoresis, and suggest instead that the particles propulsion mechanism may in fact bear close resemblance to that operative in bimetallic swimmers.

Annexins: Components of the Calcium and Reactive Oxygen Signaling Network

Despite the importance of reactive oxygen species (ROS) in plant immunity, stress signaling, and development ([Mori and Schroeder, 2004][1]; [Gadjev et al., 2006][2]), the molecular identities of Ca2+-permeable channels responding to ROS have not been established. Here, we propose annexins as

Flickering analysis of erythrocyte mechanical properties: dependence on oxygenation level, cell shape, and hydration level.

Erythrocytes (red blood cells) play an essential role in the respiratory functions of vertebrates, carrying oxygen from lungs to tissues and CO(2) from tissues to lungs. They are mechanically very soft, enabling circulation through small capillaries. The small thermally induced displacements of the membrane provide an important tool in the investigation of the mechanics of the cell membrane. However, despite numerous studies, uncertainties in the interpretation of the data, and in the values derived for the main parameters of cell mechanics, have rendered past conclusions from the fluctuation approach somewhat controversial. Here we revisit the experimental method and theoretical analysis of fluctuations, to adapt them to the case of cell contour fluctuations, which are readily observable experimentally. This enables direct measurements of membrane tension, of bending modulus, and of the viscosity of the cell cytoplasm. Of the various factors that influence the mechanical properties of the cell, we focus here on: 1), the level of oxygenation, as monitored by Raman spectrometry; 2), cell shape; and 3), the concentration of hemoglobin. The results show that, contrary to previous reports, there is no significant difference in cell tension and bending modulus between oxygenated and deoxygenated states, in line with the softness requirement for optimal circulatory flow in both states. On the other hand, tension and bending moduli of discocyte- and spherocyte-shaped cells differ markedly, in both the oxygenated and deoxygenated states. The tension in spherocytes is much higher, consistent with recent theoretical models that describe the transitions between red blood cell shapes as a function of membrane tension. Cell cytoplasmic viscosity is strongly influenced by the hydration state. The implications of these results to circulatory flow dynamics in physiological and pathological conditions are discussed.

Red blood cell dynamics: from spontaneous fluctuations to non-linear response

We studied experimentally the mechanical properties of the red blood cell. By attaching beads biochemically on the cell membrane at diametrically opposite positions, the membrane movements can be detected very accurately, and a deformation of the cell can be imposed. A measurement of the mechanical properties at very small amplitudes is obtained by fluctuation analysis, and compared to the stiffness at larger deformations, obtained by stretching the cellsviaoptical traps whilst monitoring the force. The cells are also probed at various conditions of pre-strain. These measurements show clearly a stiffening with strain and with pre-strain, which is strongest at low frequencies of deformation. The cell is measured to be slightly softer from fluctuation analysis, but consistent simply with the fact that the oscillation amplitude in fluctuations is very small. There is no evidence in these experiments of non-thermal sources of membrane motion, although non-thermal noise may be present within experimental error.

Swimming in a crystal

We study catalytic Janus particles and Escherichia coli bacteria swimming in a two-dimensional colloidal crystal. The Janus particles orbit individual colloids and hop between colloids stochastically, with a hopping rate that varies inversely with fuel (hydrogen peroxide) concentration. At high fuel concentration, these orbits are stable for 100s of revolutions, and the orbital speed oscillates periodically as a result of hydrodynamic, and possibly also phoretic, interactions between the swimmer and the six neighbouring colloids. Motile E. coli bacteria behave very differently in the same colloidal crystal: their circular orbits on plain glass are rectified into long, straight runs, because the bacteria are unable to turn corners inside the crystal.

Particle-size effects in the formation of bicontinuous Pickering emulsions

We demonstrate that the formation of bicontinuous emulsions stabilized by interfacial particles (bijels) is more robust when nanoparticles rather than microparticles are used. Emulsification via spinodal demixing in the presence of nearly neutrally wetting particles is induced by rapid heating. Using confocal microscopy, we show that nanospheres allow successful bijel formation at heating rates two orders of magnitude slower than is possible with microspheres. In order to explain our results, we introduce the concept of mechanical leeway, i.e., nanoparticles benefit from a smaller driving force towards disruptive curvature. Finally, we suggest that leeway mechanisms may benefit any formulation in which challenges arise due to tight restrictions on a pivotal parameter, but where the restrictions can be relaxed by rationally changing the value of a more accessible parameter.

Hydrodynamic oscillations and variable swimming speed in squirmers close to repulsive walls

We present a lattice Boltzmann study of the hydrodynamics of a fully resolved squirmer, confined in a slab of fluid between two no-slip walls. We show that the coupling between hydrodynamics and short-range repulsive interactions between the swimmer and the surface can lead to hydrodynamic trapping of both pushers and pullers at the wall, and to hydrodynamic oscillations in the case of a pusher. We further show that a pusher moves significantly faster when close to a surface than in the bulk, whereas a puller undergoes a transition between fast motion and a dynamical standstill according to the range of the repulsive interaction. Our results critically require near-field hydrodynamics and demonstrate that far-field hydrodynamics is insufficient to give even a qualitatively correct account of swimmer behaviour near walls. Finally our simulations suggest that it should be possible to control the density and speed of squirmers at a surface by tuning the range of steric and electrostatic swimmer-wall interactions.

Absolute quantification of protein copy number using a single-molecule-sensitive microarray

We report the use of a microfluidic microarray incorporating single molecule detection for the absolute quantification of protein copy number in solution. In this paper we demonstrate protocols which enable calibration free detection for two protein detection assays. An EGFP protein assay has a limit of detection of <30 EGFP proteins in a microfluidic analysis chamber (limited by non-specific background binding), with a measured limit of linearity of approximately 6 × 10(6) molecules of analyte in the analysis chamber and a dynamic range of >5 orders of magnitude in protein concentration. An antibody sandwich assay was used to detect unlabelled human tumour suppressor protein p53 with a limit of detection of approximately 21 p53 proteins and a dynamic range of >3 orders of magnitude. We show that these protocols can be used to calibrate data retrospectively to determine the absolute protein copy number at the single cell level in two human cancer cell lines.

The secret life of Pickering emulsions: particle exchange revealed using two colours of particle

Emulsion droplets stabilised by colloidal particles (Pickering emulsions) can be highly stable, so it is unsurprising that they are beginning to be exploited industrially. The individual colloidal particles have interfacial attachment energies that are vastly larger than the thermal energy, hence they are usually thought of as being irreversibly adsorbed. Here we show, for the first time, particles being exchanged between droplets in a Pickering emulsion. This occurs when the emulsion contains droplets that share particles, often called bridging. By starting with two emulsions showing bridging, each stabilised by a different colour of particle, the dynamics can be studied as they are gently mixed together on a roller bank. We find that particle exchange occurs by two routes: firstly, during a period of unbridging and rebridging whose duration can be tuned by varying the wettability of the particles, and secondly, during very rare events when particles are ejected from one droplet and re-adsorbed onto another.

Solid microscopic rings formed via wetting and subsequent dewetting

We report the spontaneous formation of rings when a colloidal dispersion, containing silica-coated iron-oxide particles and the liquids ethanol and ethoxylated trimethylolpropane triacrylate, is deposited within micron-sized PDMS wells. Just after filling, the interface between air and the dispersion is a meniscus dictated by the dispersions contact angle on PDMS. Upon evaporation of ethanol the meniscus lowers and, if a critical volume is reached, a rupture process is initiated and the dispersion adopts a ring morphology. The final dispersion consists only of particles and ethoxylated trimethylolpropane triacrylate that can be reticulated to solidify the ring geometry. The colloidal particles within the dispersion are essential for the stability of the rings prior to the reticulation. Here, by using iron-oxide based colloidal particles we fabricated superparamagnetic rings, opening up new avenues for applications. The dimensions of the rings can be tuned by adjusting both the size of the PDMS wells and the amount of ethanol in the dispersion. In this manner it is possible to fabricate rings with annuli smaller than a micron – a scale below the lower limit of standard lithography. Calculations assuming an equilibrium contact angle of ethoxylated trimethylolpropane triacrylate on PDMS reproduce the experimental results strikingly well.