Colloidal particles equipped with platinum patches can establish chemical gradients in H 2 O 2 -enriched solutions and undergo self-propulsion due to local diffusiophoretic migration. In bulk (3D), this class of active particles swim in the direction of the surface heterogeneities introduced by the patches and consequently reorient with the characteristic rotational diffusion time of the colloids. In this article, we present experimental and numerical evidence that planar 2D confinements defy this simple picture. Instead, the motion of active particles both on solid substrates and at flat liquid-liquid interfaces is captured by a 2D active Brownian motion model, in which rotational and translational motion are constrained in the xy-plane. This leads to an active motion that does not follow the direction of the surface heterogeneities and to timescales of reorientation that do not match the free rotational diffusion times. Furthermore, 2D-confinement at fluid-fluid interfaces gives rise to a unique distribution of swimming velocities: the patchy colloids uptake two main orientations leading to two particle populations with velocities that differ up to one order of magnitude. Our results shed new light on the behavior of active colloids in 2D, which is of interest for modeling and applications where confinements are present. Main textSelf-propelling colloidal particles, originally inspired to mimic living microorganims, offer exciting opportunities to engineer smart active materials [1]. Amongst them, catalytic microswimmers have for instance been realized using Janus particles [2][3][4][5]. These are colloidal particles (e.g., silica spheres) equipped with a surface patch (e.g., a platinum coating) that can catalyze the chemical reaction of a 'fuel' present in the medium (e.g., H 2 O 2 decomposed into H 2 O and O 2 ), leading to an asymmetric chemical gradient around the particles and subsequent propulsion by phoretic forces [6].The magnitude of the swimming velocity for a single particle, V, is given by the local fuel concentration [2]. The direction of motion is along the asymmetry axis of the particle (i.e. the axis that links the poles of the two different surface portions of a spherical Janus particle) and reorients with a characteristic time τ set by the particle size, the solvent viscosity and thermal energy [2,7]. Importantly, in the absence of gravitational effects [8] or interactions with confinements [9][10][11], the unit vector representing the direction of motion is allowed to freely diffuse on the surface of a unit sphere, so that reorientation occurs in 3D. Therefore, the resulting selfpropelled motion can be described by a 3D active Brownian motion model [12,13].V and τ are responsible for complex phenomena including clustering [14,15], active self-assembly [16, 17] and swarming [18], and can be altered using external fields (e.g. magnetic [19] and optical [20,21]) or by modifying the swimmer's geometry [22][23][24][25]. However, this simple picture is strictly valid only for freeswimming ...
We study the electrocaloric (EC) effect in bulk BaTiO3 (BTO) using molecular dynamics simulations of a first principles-based effective Hamiltonian, combined with direct measurements of the adiabatic EC temperature change in BTO single crystals. We examine in particular the dependence of the EC effect on the direction of the applied electric field at all three ferroelectric transitions, and we show that the EC response is strongly anisotropic. Most strikingly, an inverse caloric effect, i.e., a temperature increase under field removal, can be observed at both ferroelectric-ferroelectric transitions for certain orientations of the applied field. Using the generalized Clausius-Clapeyron equation, we show that the inverse effect occurs exactly for those cases where the field orientation favors the higher temperature/higher entropy phase. Our simulations show that temperature changes of around 1 K can in principle be obtained at the tetragonal-orthorhombic transition close to room temperature, even for small applied fields, provided that the applied field is strong enough to drive the system across the first order transition line. Our direct EC measurements for BTO single crystals at the cubic-tetragonal and at the tetragonal-orthorhombic transitions are in good qualitative agreement with our theoretical predictions, and in particular confirm the occurrence of an inverse EC effect at the tetragonal-orthorhombic transition for electric fields applied along the [001] pseudo-cubic direction.
Interfacial rheology becomes important when surface active species such as surfactants, particles, or proteins are present in sufficient quantities at liquid-liquid interfaces and interact between them. Interfacial rheometry measurements are challenging for various reasons. The mechanical response of the thin interface is often weaker compared to that of bulk materials and so one is often measuring close to the lower force and torque limits of rheometers, hence signal-to-noise ratios merit closer attention. In addition, the role of both instrument and sample inertia is more important for interfacial rheometry compared to bulk rheometry. Effects of misalignment and imperfections of the measurement geometries lead to effects of surface and line tension. Finally, peculiar for interfacial rheometry is the need to deconvolute the contributions of flow and deformation in the surrounding phases from that at the interface. Whereas some of these aspects have received attention in previous works, a clear and unambiguous view on the operating limits of interfacial rheometers has been missing. In the present work, we investigate the different experimental challenges and develop a generic methodology, which provides a clear definition of the operating limits of various interfacial rheometers including the interfacial needle shear rheometer, the double wall ring, and the bicone geometries. We validate this methodology by investigating the limitations defined intrinsically by the instrument as well as the ones emerging from the properties of the interface of interest for an interface composed of fatty alcohols which represents a challenging test case. The results provide cautionary examples and clear guidelines for anyone measuring interfacial rheology with these direct rheological techniques.
We study experimentally and numerically the motion of a self-phoretic active particle in two-dimensional loosely packed colloidal crystals at fluid interfaces. Two scenarios emerge depending on the interactions between the active particle and the lattice: the active particle either navigates throughout the crystal as an interstitial or is part of the lattice and behaves as an active atom. Active interstitials undergo a run-and-tumble-like motion, with the passive colloids of the crystal acting as tumbling sites. Instead, active atoms exhibit an intermittent motion, stemming from the interplay between the periodic potential landscape of the passive crystal and the particle's self-propulsion. Our results constitute the first step towards the realization of non-close-packed crystalline phases with internal activity.
Foams can resist destabilizaton in ways that appear similar on a macroscopic scale, but the microscopic origins of the stability and the loss thereof can be quite diverse. Here, we compare both the macroscopic drainage and ultimate collapse of aqueous foams stabilized by either a partially hydrolyzed poly(vinyl alcohol) (PVA) or a nonionic low-molecular-weight surfactant (BrijO10) with the dynamics of individual thin films at the microscale. From this comparison, we gain significant insight regarding the effect of both surface stresses and intermolecular forces on macroscopic foam stability. Distinct regimes in the lifetime of the foams were observed. Drainage at early stages is controlled by the different stress-boundary conditions at the surfaces of the bubbles between the polymer and the surfactant. The stress-carrying capacity of PVA-stabilized interfaces is a result of the mutual contribution of Marangoni stresses and surface shear viscosity. In contrast, surface shear inviscidity and much weaker Marangoni stresses were observed for the nonionic surfactant surfaces, resulting in faster drainage times, both at the level of the single film and the macroscopic foam. At longer times, the PVA foams present a regime of homogeneous coalescence where isolated coalescence events are observed. This regime, which is observed only for PVA foams, occurs when the capillary pressure reaches the maximum disjoining pressure. A final regime is then observed for both systems where a fast coalescence front propagates from the top to the bottom of the foams. The critical liquid fractions and capillary pressures at which this regime is obtained are similar for both PVA and BrijO10 foams, which most likely indicates that collapse is related to a universal mechanism that seems unrelated to the stabilizer interfacial dynamics.
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