Critical Casimir forces in soft matter.

We review recent advances in the theoretical, numerical, and experimental studies of critical Casimir forces in soft matter, with particular emphasis on their relevance for the structures of colloidal suspensions and on their dynamics. Distinct from other interactions which act in soft matter, such as electrostatic and van der Waals forces, critical Casimir forces are effective interactions characterised by the possibility to control reversibly their strength via minute temperature changes, while their attractive or repulsive character is conveniently determined via surface treatments or by structuring the involved surfaces. These features make critical Casimir forces excellent candidates for controlling the equilibrium and dynamical properties of individual colloids or colloidal dispersions as well as for possible applications in micro-mechanical systems. In the past 25 years a number of theoretical and experimental studies have been devoted to investigating these forces primarily under thermal equilibrium conditions, while their dynamical and non-equilibrium behaviour is a largely unexplored subject open for future investigations.

Structure of liquid-vapor interfaces: Perspectives from liquid state theory, large-scale simulations, and potential grazing-incidence x-ray diffraction.

Grazing-incidence x-ray diffraction (GIXRD) is a scattering technique that allows one to characterize the structure of fluid interfaces down to the molecular scale, including the measurement of surface tension and interface roughness. However, the corresponding standard data analysis at nonzero wave numbers has been criticized as to be inconclusive because the scattering intensity is polluted by the unavoidable scattering from the bulk. Here, we overcome this ambiguity by proposing a physically consistent model of the bulk contribution based on a minimal set of assumptions of experimental relevance. To this end, we derive an explicit integral expression for the background scattering, which can be determined numerically from the static structure factors of the coexisting bulk phases as independent input. Concerning the interpretation of GIXRD data inferred from computer simulations, we extend the model to account also for the finite sizes of the bulk phases, which are unavoidable in simulations. The corresponding leading-order correction beyond the dominant contribution to the scattered intensity is revealed by asymptotic analysis, which is characterized by the competition between the linear system size and the x-ray penetration depth in the case of simulations. Specifically, we have calculated the expected GIXRD intensity for scattering at the planar liquid-vapor interface of Lennard-Jones fluids with truncated pair interactions via extensive, high-precision computer simulations. The reported data cover interfacial and bulk properties of fluid states along the whole liquid-vapor coexistence line. A sensitivity analysis shows that our findings are robust with respect to the detailed definition of the mean interface position. We conclude that previous claims of an enhanced surface tension at mesoscopic scales are amenable to unambiguous tests via scattering experiments.

Pumping and Mixing in Active Pores.

We show both numerically and analytically that a chemically patterned active pore can act as a micro- or nanopump for fluids, even if it is fore-aft symmetric. This is possible due to a spontaneous symmetry breaking which occurs when advection rather than diffusion is the dominant mechanism of solute transport. We further demonstrate that, for pumping and tuning the flow rate, a combination of geometrical and chemical inhomogeneities is required. For certain parameter values, the flow is unsteady, and persistent oscillations with a tunable frequency appear. Finally, we find that the flow exhibits convection rolls and hence promotes mixing in the low Reynolds number regime.

Motion adaptation improves acuity (but perceived size doesn't matter).

Recognition acuity-the minimum size of a high-contrast object that allows us to recognize it-is limited by optical and neural elements of the eye and by processing within the visual cortex. The perceived size of objects can be changed by motion-adaptation. Viewing receding or looming motion makes subsequently viewed stimuli appear to grow or shrink, respectively. It has been reported that resulting changes in perceived size impact recognition acuity. We set out to determine if such acuity changes are reliable and what drives this phenomenon. We measured the effect of adaptation to receding and looming motion on acuity for crowded tumbling-T stimuli (). We quantified the role of crowding, individuals' susceptibility to motion-adaptation, and potentially confounding effects of pupil size and eye movements. Adaptation to receding motion made targets appear larger and improved acuity (-0.037 logMAR). Although adaptation to looming motion made targets appear smaller, it induced not the expected decrease in acuity but a modest acuity improvement (-0.018 logMAR). Further, each observer's magnitude of acuity change was not correlated with their individual perceived-size change following adaptation. Finally, we found no evidence that adaptation-induced acuity gains were related to crowding, fixation stability, or pupil size. Adaptation to motion modestly enhances visual acuity, but unintuitively, this is dissociated from perceived size. Ruling out fixation and pupillary behavior, we suggest that motion adaptation may improve acuity via incidental effects on sensitivity-akin to those arising from blur adaptation-which shift sensitivity to higher spatial frequency-tuned channels.

The role of counterions in ionic liquid crystals.

Previous theoretical studies of calamitic (i.e., rod-like) ionic liquid crystals (ILCs) based on an effective one-species model led to indications of a novel smectic-A phase with a layer spacing being much larger than the length of the mesogenic (i.e., liquid-crystal forming) ions. In order to rule out the possibility that this wide smectic-A phase is merely an artifact caused by the one-species approximation, we investigate an extension that accounts explicitly for cations and anions in ILCs. Our present findings, obtained by grand canonical Monte Carlo simulations, show that the phase transitions between the isotropic and the smectic-A phases of the cation-anion system are in qualitative agreement with the effective one-species model used in the preceding studies. In particular, for ILCs with mesogens (i.e., liquid-crystal forming species) carrying charged sites at their tips, the wide smectic-A phase forms, at low temperatures and within an intermediate density range, in between the isotropic and hexagonal crystal phases. We find that in the ordinary smectic-A phase, the spatial distribution of the counterions of the mesogens is approximately uniform, whereas in the wide smectic-A phase, the small counterions accumulate in between the smectic layers. Due to this phenomenology, the wide smectic-A phase could be interesting for applications, which hinge on the presence of conductivity channels for mobile ions.

Liquid-liquid phase separation in an inhomogeneous ternary colloid-polymer mixture.

Suspended colloids are often considered as models for molecules, which are sufficiently big so that they can be observed directly in (light) microscopes and for which the effective interaction among each other can be tailored. The Asakura-Oosawa model of ideal colloid-polymer mixtures captures the idea of tuning the interaction between the colloids via a potential, which possesses a range set by the size of the polymers and an attractive strength characterized by the (reservoir) number density of the polymers, which plays the role of an inverse temperature. The celebrated Asakura-Oosawa depletion potential allows one to recreate the bulk phase diagram of a simple fluid by employing a colloid-polymer mixture. This has been verified in theory, by computer simulations, and via experiments. Here, we study the phase behavior of a confined colloid-polymer mixture with two polymer species. The sizes and densities are chosen such that the resulting bulk phase diagram exhibits a second stable critical point within the framework of the classical density functional theory. Our results suggest that a suitably tuned colloid-polymer mixture can be an interesting model system to study fluids with two critical points.

Self-Motility of an Active Particle Induced by Correlations in the Surrounding Solution.

Current models of phoretic transport rely on molecular forces creating a "diffuse" particle-fluid interface. We investigate theoretically an alternative mechanism, in which a diffuse interface emerges solely due to a nonvanishing correlation length of the surrounding solution. This mechanism can drive self-motility of a chemically active particle. Numerical estimates indicate that the velocity can reach micrometers per second. The predicted phenomenology includes a bilinear dependence of the velocity on the activity and a possible double velocity reversal upon varying the correlation length.

Correction: Transient coarsening and the motility of optically heated Janus colloids in a binary liquid mixture.

Correction for 'Transient coarsening and the motility of optically heated Janus colloids in a binary liquid mixture' by Juan Ruben Gomez-Solano et al., Soft Matter, 2020, DOI: 10.1039/d0sm00964d.

Transient coarsening and the motility of optically heated Janus colloids in a binary liquid mixture.

A gold-capped Janus particle suspended in a near-critical binary liquid mixture can self-propel under illumination. We have immobilized such a particle in a narrow channel and carried out a combined experimental and theoretical study of the non-equilibrium dynamics of a binary solvent around it - lasting from the very moment of switching illumination on until the steady state is reached. In the theoretical study we use both a purely diffusive and a hydrodynamic model, which we solve numerically. Our results demonstrate a remarkable complexity of the time evolution of the concentration field around the colloid. This evolution is governed by the combined effects of the temperature gradient and the wettability, and crucially depends on whether the colloid is free to move or is trapped. For the trapped colloid, all approaches indicate that the early time dynamics is purely diffusive and characterized by composition layers travelling with constant speed from the surface of the colloid into the bulk of the solvent. Subsequently, hydrodynamic effects set in. Anomalously large nonequilibrium fluctuations, which result from the temperature gradient and the vicinity of the critical point of the binary liquid mixture, give rise to strong concentration fluctuations in the solvent and to permanently changing coarsening patterns not observed for a mobile particle. The early time dynamics around initially still Janus colloids produces a force which is able to set the Janus colloid into motion. The propulsion due to this transient dynamics is in the direction opposite to that observed after the steady state is attained.

Numerical simulations of self-diffusiophoretic colloids at fluid interfaces.

The dynamics of active colloids is very sensitive to the presence of boundaries and interfaces which therefore can be used to control their motion. Here we analyze the dynamics of active colloids adsorbed at a fluid-fluid interface. By using a mesoscopic numerical approach which relies on an approximated numerical solution of the Navier-Stokes equation, we show that when adsorbed at a fluid interface, an active colloid experiences a net torque even in the absence of a viscosity contrast between the two adjacent fluids. In particular, we study the dependence of this torque on the contact angle of the colloid with the fluid-fluid interface and on its surface properties. We rationalize our results via an approximate approach which accounts for the appearance of a local friction coefficient. By providing insight into the dynamics of active colloids adsorbed at fluid interfaces, our results are relevant for two-dimensional self assembly and emulsion stabilization by means of active colloids.

Finite-size corrections for the static structure factor of a liquid slab with open boundaries.

The presence of a confining boundary can modify the local structure of a liquid markedly. In addition, small samples of finite size are known to exhibit systematic deviations of thermodynamic quantities relative to their bulk values. Here, we consider the static structure factor of a liquid sample in slab geometry with open boundaries at the surfaces, which can be thought of as virtually cutting out the sample from a macroscopically large, homogeneous fluid. This situation is a relevant limit for the interpretation of grazing-incidence diffraction experiments at liquid interfaces and films. We derive an exact, closed expression for the slab structure factor, with the bulk structure factor as the only input. This shows that such free boundary conditions cause significant differences between the two structure factors, in particular, at small wavenumbers. An asymptotic analysis of this result yields the scaling exponent and an accurate, useful approximation of these finite-size corrections. Furthermore, the open boundaries permit the interpretation of the slab as an open system, supporting particle exchange with a reservoir. We relate the slab structure factor to the particle number fluctuations and discuss conditions under which the subvolume of the slab represents a grand canonical ensemble with chemical potential µ and temperature T. Thus, the open slab serves as a test-bed for the small-system thermodynamics in a µT reservoir. We provide a microscopically justified and exact result for the size dependence of the isothermal compressibility. Our findings are corroborated by simulation data for Lennard-Jones liquids at two representative temperatures.

Effective pair interaction of patchy particles in critical fluids.

We study the critical Casimir interaction between two spherical colloids immersed in a binary liquid mixture close to its critical demixing point. The surface of each colloid prefers one species of the mixture with the exception of a circular patch of arbitrary size, where the other species is preferred. For such objects, we calculate, within the Derjaguin approximation, the scaling function describing the critical Casimir potential, and we use it to derive the scaling functions for all components of the forces and torques acting on both colloids. The results are compared with available experimental data. Moreover, the general relation between the scaling function for the potential and the scaling functions for the force and the torque is derived.

Heterogeneous surface charge confining an electrolyte solution.

The structure of dilute electrolyte solutions close to a surface carrying a spatially inhomogeneous surface charge distribution is investigated by means of classical density functional theory within the approach of fundamental measure theory. For electrolyte solutions, the influence of these inhomogeneities is particularly strong because the corresponding characteristic length scale is the Debye length, which is large compared to molecular sizes. Here, a fully three-dimensional investigation is performed, which accounts explicitly for the solvent particles, and thus provides insight into effects caused by ion-solvent coupling. The present study introduces a versatile framework to analyze a broad range of types of surface charge heterogeneities even beyond the linear response regime. This reveals a sensitive dependence of the number density profiles of the fluid components and of the electrostatic potential on the magnitude of the charge as well as on the details of the surface charge patterns at small scales.

Bridging transitions and capillary forces for colloids in a slit.

Capillary bridges can form between colloids immersed in a two-phase fluid, e.g., in a binary liquid mixture, if the surface of the colloids prefers the species other than the one favored in the bulk liquid. Here, we study the formation of liquid bridges induced by confining colloids to a slit, with the slit walls having a preference opposite to the one of the colloid surface. Using mean field theory, we show that there is a line of first-order phase transitions between the bridge and the no-bridge states, which ends at a critical point. By decreasing the slit width, this critical point is shifted toward smaller separations between the colloids. However, at very small separations and far from criticality, we observe only a minor influence of the slit width on the location of the transition. Monte Carlo simulations of the Ising model, which mimics incompressible binary liquid mixtures, confirm the occurrence of the bridging transitions, as manifested by the appearance of "spinodal" regions where both bridge and no-bridge configurations are stable or metastable. Interestingly, we find that there is no such spinodal region in the case of small colloids, but we observe a sharpening of the transition when the colloid size increases. In addition, we demonstrate that the capillary force acting between the colloids can depend sensitively on the slit width and varies drastically with temperature, thus achieving strengths orders of magnitude higher than at criticality of the fluid.

High-Quality Magnetotransport in Graphene Using the Edge-Free Corbino Geometry.

We report fabrication of graphene devices in a Corbino geometry consisting of concentric circular electrodes with no physical edge connecting the inner and outer electrodes. High device mobility is realized using boron nitride encapsulation together with a dual-graphite gate structure. Bulk conductance measurement in the quantum Hall effect (QHE) regime outperforms previously reported Hall bar measurements, with improved resolution observed for both the integer and fractional QHE states. We identify apparent phase transitions in the fractional sequence in both the lowest and first excited Landau levels (LLs) and observe features consistent with electron solid phases in higher LLs.

Dynamics near planar walls for various model self-phoretic particles.

For chemically active particles suspended in a liquid solution and moving by self-phoresis, the dynamics near chemically inert, planar walls is studied theoretically by employing various choices for the activity function, i.e., the spatial distribution of the sites where various chemical reactions take place. We focus on the case of solutions composed of electrically neutral species. This analysis extends previous studies of the case that the chemical activity can be modeled effectively as the release of a "product" molecular species from parts of the surface of the particle by accounting for annihilation of the product molecules by chemical reactions, either on the rest of the surface of the particle or in the volume of the surrounding solution. We show that, for the models considered here, the emergence of "sliding" and "hovering" wall-bound states is a generic, robust feature. However, the details of these states, such as the range of parameters within which they occur, depend on the specific model for the activity function. Additionally, in certain cases there is a reversal of the direction of the motion compared to the one observed if the particle is far away from the wall. We have also studied the changes of the dynamics induced by a direct interaction between the particle and the wall by including a short-ranged repulsive component to the interaction in addition to the steric one (a procedure often employed in numerical simulations of active colloids). Upon increasing the strength of this additional component, while keeping its range fixed, significant qualitative changes occur in the phase portraits of the dynamics near the wall: for sufficiently strong short-ranged repulsion, the sliding steady states of the dynamics are transformed into hovering states. Furthermore, our studies provide evidence for an additional "oscillatory" wall-bound steady state of motion for chemically active particles due to a strong, short-ranged, and direct repulsion. This kind of particle translates along the wall at a distance from it which oscillates between a minimum and a maximum.

Active Janus colloids at chemically structured surfaces.

If catalytically active Janus particles are dispersed in certain liquid solutions, they can create a gradient in the chemical composition of this solution along their surfaces, as well as along any nearby confining surfaces. This gradient drives self-propulsion via a self-phoretic mechanism, while the compositional gradient along a wall gives rise to chemiosmosis, which additionally contributes to self-motility. In this study, we analyze theoretically the dynamics of an active colloid near chemically patterned walls. We use a point-particle approximation combined with a multipole expansion in order to discuss the effects of pattern geometry and chemical contrast on the particle trajectories. In particular, we consider planar walls patterned with chemical steps and stripes. We investigate in detail the changes in the topology of the corresponding phase portraits upon varying the chemical contrast and the stripe width.

Assessing cognitive dysfunction in Parkinson's disease: An online tool to detect visuo-perceptual deficits.

BACKGROUND: People with Parkinson's disease (PD) who develop visuo-perceptual deficits are at higher risk of dementia, but we lack tests that detect subtle visuo-perceptual deficits and can be performed by untrained personnel. Hallucinations are associated with cognitive impairment and typically involve perception of complex objects. Changes in object perception may therefore be a sensitive marker of visuo-perceptual deficits in PD. OBJECTIVE: We developed an online platform to test visuo-perceptual function. We hypothesised that (1) visuo-perceptual deficits in PD could be detected using online tests, (2) object perception would be preferentially affected, and (3) these deficits would be caused by changes in perception rather than response bias. METHODS: We assessed 91 people with PD and 275 controls. Performance was compared using classical frequentist statistics. We then fitted a hierarchical Bayesian signal detection theory model to a subset of tasks. RESULTS: People with PD were worse than controls at object recognition, showing no deficits in other visuo-perceptual tests. Specifically, they were worse at identifying skewed images (P < .0001); at detecting hidden objects (P = .0039); at identifying objects in peripheral vision (P < .0001); and at detecting biological motion (P = .0065). In contrast, people with PD were not worse at mental rotation or subjective size perception. Using signal detection modelling, we found this effect was driven by change in perceptual sensitivity rather than response bias. CONCLUSIONS: Online tests can detect visuo-perceptual deficits in people with PD, with object recognition particularly affected. Ultimately, visuo-perceptual tests may be developed to identify at-risk patients for clinical trials to slow PD dementia. © 2018 The Authors. Movement Disorders published by Wiley Periodicals, Inc. on behalf of International Parkinson and Movement Disorder Society.

Electrostatic interaction of particles trapped at fluid interfaces: effects of geometry and wetting properties.

The electrostatic interaction between pairs of spherical or macroscopically long, parallel cylindrical colloids trapped at fluid interfaces is studied theoretically for the case of small inter-particle separations. Starting from the effective interaction between two planar walls and by using the Derjaguin approximation, we address the issue of how the electrostatic interaction between such particles is influenced by their curvatures and by the wetting contact angle at their surfaces. Regarding the influence of curvature, our findings suggest that the discrepancies between linear and nonlinear Poisson-Boltzmann theory, which have been noticed before for planar walls, also occur for spheres and macroscopically long, parallel cylinders, though their magnitude depends on the wetting contact angle. Concerning the influence of the wetting contact angle θ simple relations are obtained for equally sized particles which indicate that the inter-particle force varies significantly with θ only within an interval around 90°. This interval depends on the Debye length of the fluids and on the size of the particles but not on their shape. For unequally sized particles, a more complicated relation is obtained for the variation of the inter-particle force with the wetting contact angle.