Thermodiffusion anisotropy under a magnetic field in ionic liquid-based ferrofluids.

Ferrofluids based on maghemite nanoparticles (NPs), typically 10 nm in diameter, are dispersed in an ionic liquid (1-ethyl 3-methylimidazolium bistriflimide - EMIM-TFSI). The average interparticle interaction is found to be repulsive by small angle scattering of X-rays and of neutrons, with a second virial coefficient A2 = 7.3. A moderately concentrated sample at Φ = 5.95 vol% is probed by forced Rayleigh scattering under an applied magnetic field (up to H = 100 kA m-1) from room temperature up to T = 460 K. Irrespective of the values of H and T, the NPs in this study are always found to migrate towards the cold region. The in-field anisotropy of the mass diffusion coefficient Dm and that of the (always positive) Soret coefficient ST are well described by the presented model in the whole range of H and T. The main origin of anisotropy is the spatial inhomogeneities of concentration in the ferrofluid along the direction of the applied field. Since this effect originates from the magnetic dipolar interparticle interaction, the anisotropy of thermodiffusion progressively vanishes when temperature and thermal motion increase.

Thermodiffusion of citrate-coated γ-Fe2O3 nanoparticles in aqueous dispersions with tuned counter-ions - anisotropy of the Soret coefficient under a magnetic field.

Under a temperature gradient, the direction of thermodiffusion of charged γ-Fe2O3 nanoparticles (NPs) depends on the nature of the counter-ions present in the dispersion, resulting in either a positive or negative Soret coefficient. Various counter-ions are probed in finely tuned and well characterized dispersions of citrate-coated NPs at comparable concentrations of free ionic species. The Soret coefficient ST is measured in stationary conditions together with the mass-diffusion coefficient Dm using a forced Rayleigh scattering method. The strong interparticle repulsion, determined by SAXS, is also attested by the increase of Dm with NP volume fraction Φ. The Φ-dependence of ST is analyzed in terms of thermophoretic and thermoelectric contributions of the various ionic species. The obtained single-particle thermophoretic contribution of the NPs (the Eastman entropy of transfer sNP) varies linearly with the entropy of transfer of the counter-ions. This is understood in terms of electrostatic contribution and of hydration of the ionic shell surrounding the NPs. Two aqueous dispersions, respectively, with ST > 0 and with ST < 0 are then probed under an applied field H[combining right harpoon above], and an anisotropy of Dm and of ST is induced while the in-field system remains monophasic. Whatever the H[combining right harpoon above]-direction (parallel or perpendicular to the gradients and ), the Soret coefficient is modulated keeping the same sign as in zero applied field. In-field experimental determinations are well described using a mean field model of the interparticle magnetic interaction.

Gravity effects on mixing with magnetic micro-convection in microfluidics.

Mixing remains an important problem for the development of successful microfluidic and lab-on-a-chip devices, where simple and predictable systems are particularly interesting. One is magnetic micro-convection, an instability happening on the interface of miscible magnetic and non-magnetic fluids in a Hele-Shaw cell under applied field. Previous work proved that the Brinkman model quantitatively explains the experiments. However, a gravity-caused convective motion complicated the tests. Here we first improve the experimental system to exclude the parasitic convection. Afterwards, we experimentally observe the magnetic micro-convection, by finding and quantifying how gravity and laminar flow stabilizes the perturbations that create it. Accordingly, we improve our theoretical model for a zero-flow condition and perform a linear analysis. Two dimensionless quantities --magnetic and gravitational Rayleigh numbers-- are used to compare the experimental observations and theoretical predictions for the critical field of instability and the characteristic size of the emerging pattern. Finally, we discuss the conditions at which gravity plays an important role in microfluidic systems.

Bilayer properties of giant magnetic liposomes formed by cationic pyridine amphiphile and probed by active deformation under magnetic forces.

We synthesize giant magnetic liposomes by a reverse-phase evaporation method (REV) using a new self-assembling Cationic Pyridine Amphiphile (CPA) derived from 1,4-dihydropyridine as liposome-forming agent and a magnetic ferrofluid based on γ-Fe(2)O(3) nanoparticles. Having in view the potential interest of CPA in targeted transport by magnetic forces, the mechanical elastic properties of such bilayers are here directly investigated in vesicles loaded with magnetic nanoparticles. Bending elastic modulus K(b) ∼ 0.2 to 5k(B)T and pre-stress τ ∼ 3.2 to 12.10(-6) erg/cm(2) are deduced from the under-field deformations of the giant magnetic liposomes. The obtained K(b) values are discussed in terms of A. Wurgers's theory.

Rotating hematite cube chains.

Recently a two-dimensional chiral fluid was experimentally demonstrated. It was obtained from cubic-shaped hematite colloidal particles placed in a rotating magnetic field. Here we look at building blocks of that fluid by analyzing short hematite chain behavior in a rotating magnetic field. We find equilibrium structures of chains in static magnetic fields and observe chain dynamics in rotating magnetic fields. We find and experimentally verify that there are three planar motion regimes and one where the cube chain goes out of the plane of the rotating magnetic field. In this regime we observe interesting dynamics-the chain rotates slower than the rotating magnetic field. In order to catch up with the magnetic field, it rolls on an edge and through rotation in the third dimension catches up with the magnetic field. The same dynamics is also observable for a single cube when gravitational effects are explicitly taken into account.

Equilibrium shapes and stability of magnetic filaments.

Equilibrium shapes of magnetic rods and their stability under the action of an applied field are analyzed. The family of shapes is characterized by two magnetoelastic numbers due to the remanent magnetization and paramagnetic susceptibility of the rod. Since in experiments with flexible magnetic rods the ends are usually unfixed and unclamped, their stability is analyzed under these conditions. Solutions of the corresponding eigenvalue problems for particular cases show that under these conditions the equilibrium shapes are unstable.

Energetically favorable configurations of hematite cube chains.

Hematite at room temperature is a weak ferromagnetic material. Its permanent magnetization is three orders smaller than for magnetite. Thus, hematite colloids allow us to explore a different physical range of particle interaction parameters compared to ordinary ferromagnetic particle colloids. In this paper we investigate a colloid consisting of hematite particles with cubic shape. We search for energetically favorable structures in an external magnetic field with analytical and numerical methods and molecular dynamics simulations and analyze whether it is possible to observe them in experiments. We find that energetically favorable configurations are observable only for short chains. Longer chains usually contain kinks which are formed in the process of chain formation due to the interplay of energy and thermal fluctuations as an individual cube can be in one of two alignments with an equal probability.

Dynamics of superparamagnetic filaments with finite magnetic relaxation time.

In this paper we formulate a model of superparamagnetic filaments with internal dissipative torques due to the action of a rotating magnetic field. It is shown that spirals are formed at both ends of the filament due to the action of the internal torques. These spirals propagate to the center of the filament and collide, forming a compact cluster that rotates in accordance with the rotating magnetic field. These results are in agreement with recent experiments with chains of superparamagnetic beads in a rotating magnetic field.

Ferromagnetic microswimmer.

The self-propelling motion of the flexible ferromagnetic swimmer is described. Necessary symmetry breaking is achieved by the buckling instability at field inversion. The characteristics of self-propulsion are in good agreement with the numerical calculations of the Floquet multipliers for the ferromagnetic filament under the action of ac magnetic field. In the low frequency range the power stroke of self-propelling motion is similar to that used by the unicellular green algae chlamydomonas and in the high frequency region the self-propulsion is due to the undulation waves propagating from the free ends perpendicularly to ac magnetic field.

Rotating-field-driven ensembles of magnetic particles.

Vortex patterns in ensembles of magnetic particles driven by a rotating field are studied. The driving arises due to the lubrication forces between the rotating particles acting in the direction perpendicular to the radius vector between the particles. Since the lubrication forces cannot be equilibrated by the radial forces due to the dipolar attraction and steric repulsion, the ensemble is in a nonequilibrium state. Different regimes are found for the dynamics of the driven ensembles-solid-body rotation at low frequency of the rotating field and stick-slip motion of the external layers of the aggregate with respect to the internal structure as the frequency is increased. The relation obtained for describing the angular velocity of the solid-body rotation is in good agreement with existing experimental data.

Electrostatic contribution to the surface pressure of charged monolayers containing polyphosphoinositides.

Structural and functional studies of lateral heterogeneity in biological membranes have underlined the importance of membrane organization in biological function. Most inquiries have focused on steric determinants of membrane organization, such as headgroup size and acyl-chain saturation. This manuscript reports a combination of theory and experiment that shows significant electrostatic contributions to surface pressures in monolayers of phospholipids where the charge spacing is smaller than the Bjerrum length. For molecules with steric cross sections typical of phospholipids in the cell membrane (approximately 50 A(2)), only polyphosphoinositides achieve this threshold. The most abundant such lipid is phosphatidylinositol bisphosphate, which has between three and four charged groups at physiological conditions. Theory and experiment show that surface pressure increases linearly with phosphatidylinositol bisphosphate net charge and reveal crossing of high and low ionic strength pressure-area isotherms, due to opposing effects of ionic strength in compressed and expanded monolayers. Theory and experiment show that electrostatic effects are negligible for monolayers of univalent lipids, emphasizing the unique importance of electrostatic effects for lateral organization of polyphosphoinositides. Quantitative differences between theory and experiment suggest that attractive interactions between polyphosphoinositides, possibly mediated by hydrogen bonding, can lessen the effect of electrostatic repulsions.

When a crack is oriented by a magnetic field.

Upon drying, colloidal suspensions undergo a phase transformation from a "liquid" to a "gel" state. With further solvent evaporation, tensile stresses develop in the gel, which ultimately leads to fractures. These generally manifest themselves in regular cracking patterns which reflect the physical conditions of the drying process. Here we show experimentally and theoretically how, in the case of a drying droplet of magnetic colloid (ferrofluid), an externally applied magnetic field modifies the stress in the gel and therefore the crack patterns. We find that the analysis of the shape of the cracks allows one to estimate the value of the gel Young's modulus just before the crack nucleation.

Elastic properties of DNA linked flexible magnetic filaments.

Elastic properties of magnetic filaments linked by DNA in solutions of univalent and bivalent salts with different pH values are investigated through their deformation in an external field. A strong dependence of the bending modulus in bivalent salt solution on the pH is shown. Experimental results are interpreted on the basis of the magnetic elastica.

Magnetic elastica.

Magnetic elastica with spontaneous magnetization and superparamagnetic properties are considered. Obtained solutions illustrate the characteristic transformations of their shapes as spontaneous magnetization increases. Solutions are selected on the basis of the stability analysis and results of numerical simulations. A different mechanism of the magnetic relaxation in suspension of ferromagnetic filaments by migration of a loop with antiparallel to the field magnetization is predicted.

Dynamics of a flexible ferromagnetic filament in a rotating magnetic field.

Flexible magnetic filaments have garnered considerable attention as prospective materials for the creation of different microdevices. We describe a theoretical model of a ferromagnetic filament and derive its equations of motion by variational techniques. The numerical algorithm used to solve the filament dynamics in magnetic fields of different configurations is described. It is found that in a rotating field the filament transitions between synchronous and asynchronous regimes with respect to the rotating field, similarly to a rigid magnetic dipole. The mean angular velocity of the filament is well described by a relation valid for a rigid magnetic dipole with quantitative differences attributable to the flexibility of the filament.

Synchronized rotation in swarms of magnetotactic bacteria.

Self-organizing behavior has been widely reported in both natural and artificial systems, typically distinguishing between temporal organization (synchronization) and spatial organization (swarming). Swarming has been experimentally observed in systems of magnetotactic bacteria under the action of external magnetic fields. Here we present a model of ensembles of magnetotactic bacteria in which hydrodynamic interactions lead to temporal synchronization in addition to the swarming. After a period of stabilization during which the bacteria form a quasiregular hexagonal lattice structure, the entire swarm begins to rotate in a direction opposite to the direction of the rotation of the magnetic field. We thus illustrate an emergent mechanism of macroscopic motion arising from the synchronized microscopic rotations of hydrodynamically interacting bacteria, reminiscent of the recently proposed concept of swarmalators.

Dynamics of an active magnetic particle in a rotating magnetic field.

The motion of an active (self-propelling) particle with a permanent magnetic moment under the action of a rotating magnetic field is considered. We show that below a critical frequency of the external field the trajectory of a particle is a circle. For frequencies slightly above the critical point the particle moves on an approximately circular trajectory and from time to time jumps to another region of space. Symmetry of the particle trajectory depends on the commensurability of the field period and the period of the orientational motion of the particle. We also show how our results can be used to study the properties of naturally occurring active magnetic particles, so-called magnetotactic bacteria.

Dynamic fluctuations of dipolar semiflexible filaments.

On the basis of the model of a flexible magnetic filament, the characteristics of their thermal fluctuations are considered. The crossover of the time dependence of the mean quadratic displacement from t(3/4) to t(1/2) at the magnetic field increase is found. Two characteristic mechanisms of the magnetization relaxation time distribution--straightening of the thermal undulations and excitation of the bending modes of the free ends under the action of an ac magnetic field--are described. In both cases, the characteristic scaling law omega(-3/4) of the magnetic susceptibility in a high-frequency range is found.

Nonlinear dynamics of semiflexible magnetic filaments in an ac magnetic field.

Flexible spontaneously magnetized filaments exist in the living world (magnetotactic bacteria) and arise in magnetic colloids with large magnetodipolar interaction parameter. We demonstrate that these filaments possess variety of novel nonlinear phenomena in an ac magnetic field: orientation of the filament in the direction perpendicular to the field and the development of the oscillating U-like shapes, which presumably can lead to the formation of rings of magnetic filaments. It is found that these phenomena are determined by the development of the localized boundary modes of the filament deformation. We have illustrated by qualitative estimates that the phenomena found may be useful for insight into the complex pattern formation phenomena in ensembles of magnetic particles under the action of an ac magnetic field.

Hydrodynamics with spin in bacterial suspensions.

We describe a kind of self-propelling motion of bacteria based on the cooperative action of rotating flagella on the surface of bacteria. Describing the ensemble of rotating flagella in the framework of the hydrodynamics with spin, the reciprocal theorem of Stokesian hydrodynamics is generalized accordingly. The velocity of the self-propulsion is expressed in terms of the characteristics of the vector field of flagella orientation and it is shown that the unusually high velocities of Thiovulum majus bacteria may be explained by the cooperative action of the rotating flagella. The expressions obtained enable us to estimate the torque created by the rotary motors of the bacterium and show quantitative agreement with the existing experimental data.