Spherical Janus Particles Research Articles

Orbits, Spirals, and Trapped States: Dynamics of a Phoretic Janus Particle in a Radial Concentration Gradient.

A long-standing goal in colloidal active matter is to understand how gradients in fuel concentration influence the motion of phoretic Janus particles. Here, we present a theoretical description of the motion of a spherical phoretic Janus particle in the presence of a radial gradient of the chemical solute driving self-propulsion. Radial gradients are a geometry relevant to many scenarios in active matter systems and naturally arise due to the presence of a point source or sink of fuel. We derive an analytical solution for the Janus particle's velocity and quantify the influence of the radial concentration gradient on the particle's trajectory. Compared to a phoretic Janus particle in a linear gradient in fuel concentration, we uncover a much richer set of dynamic behaviors including circular orbits and trapped stationary states. We identify the ratio of the phoretic mobilities between the two domains of the Janus particle as a central quantity in tuning their dynamics. Our results provide a path for developing optimum protocols for tuning the dynamics of phoretic Janus particles and mixing fluid at the microscale. In addition, this work suggests a method for quantifying the surface properties of phoretic Janus particles, which have proven to be challenging to probe experimentally.

Self-diffusiophoretic propulsion of a spheroidal particle in a shear-thinning fluid

Shear-thinning viscosity is a non-Newtonian behaviour that active particles often encounter in biological fluids such as blood and mucus. The fundamental question of how this ubiquitous non-Newtonian rheology affects the propulsion of active particles has attracted substantial interest. In particular, spherical Janus particles driven by self-diffusiophoresis, a major physico-chemical propulsion mechanism of synthetic active particles, were shown to always swim slower in a shear-thinning fluid than in a Newtonian fluid. In this work, we move beyond the spherical limit to examine the effect of particle eccentricity on self-diffusiophoretic propulsion in a shear-thinning fluid. We use a combination of asymptotic analysis and numerical simulations to show that shear-thinning rheology can enhance self-diffusiophoretic propulsion of a spheroidal particle, in stark contrast to previous findings for the spherical case. A systematic characterization of the dependence of the propulsion speed on the particle's active surface coverage has also uncovered an intriguing feature associated with the propulsion speeds of a pair of complementarily coated particles not previously reported. Symmetry arguments are presented to elucidate how this new feature emerges as a combined effect of anisotropy of the spheroidal geometry and nonlinearity in fluid rheology.

On the Interfacial Assembly of Anisotropic Amphiphilic Janus Particles

AbstractIt has been shown both theoretically and experimentally that amphiphilic Janus particles are the most effective solid surfactants to stabilize interfaces. In most cases, the Janus particles investigated have uniform morphologies with Janus boundaries dividing the particle into halves. However, there are many examples of Janus particles where the hydrophilic and hydrophobic domains are not equally distributed. The effects of this uneven domain distribution on the mechanism and kinetics of Janus particle assembly, and final equilibrium state are not well‐understood. Dynamic pendant drop tensiometry offers a means to probe both the equilibrium assembly and the kinetics and mechanism of assembly. Here, the interfacial kinetics and assembly of spherical anisotropic Janus particles are investigated using dynamic pendant drop tensiometry. Systematic studies quantifying the time‐dependent interfacial behavior as a function of Janus particle morphology, chemical composition, particle concentration, and NaOH and HCl concentration are performed. These studies shed light on the assembly mechanism of more complex Janus particle morphologies and highlight their effectiveness as interface stabilizers.

Regime change in the aggregate structures of spherical magnetic Janus particles (quasi-2D Monte Carlo simulations)

We have investigated a suspension composed of spherical magnetic Janus particles in thermodynamic equilibrium. The magnetic moment of Janus particles treated here is located at a position shifted from the particle centre, which is on the line perpendicular to the magnetic moment direction. We conducted quasi-2D Monte Carlo simulations to investigate the change in the regime of aggregate structures and the dependence of the regime on various factors, such as the strength of the magnetic particle-particle interaction, magnetic particle-field interaction, and the distance of the magnetic moment from the particle centre. In the absence of an applied magnetic field, the Janus particles aggregate to form stable clusters composed of a few particles with increased values of the magnetic particle-particle interaction strength. As the strength of the magnetic field is increased, these clusters collapse, and chain-like clusters are formed aligned in the direction of the magnetic field. The appearance of this regime change requires a stronger magnetic field as the position of the magnetic moment approaches the particle surface. This can be attributed to the fact that the magnetic interaction between neighbouring particles becomes more dominant as the magnetic moments of the constituent particles in the cluster units approach each other. Highlights We have addressed the aggregation phenomena in a suspension composed of spherical magnetic Janus particles. We have investigated the regime change in the aggregate structures of the Janus particles under various conditions. In a strong magnetic field, thick chain-like clusters are formed as the magnetic moment is shifted away from the particle centre. The present results are useful for elucidating the internal structure of complex aggregates in 3D systems.

Impact of the Electric Polarizability on the Transport and Collective Dynamics of Metallodielectric Janus Particles.

The objective of this article is to investigate how the electric polarizability manifests on the propulsion and collective dynamics of metallodielectric Janus particles by comparing the velocity spectra under rotating and nonrotating AC fields. Janus particles were fabricated by depositing sequential layers of titanium and SiO2 on spherical cores. Model systems of known polarizability were created by varying the thickness of titanium or by adjusting the concentration of electrolyte. We found that the spectra for propulsion velocity displayed features (amplitude and transition frequencies) that were closely matched in the electrorotation spectra. That is, the transition frequency from dielectric- to metal-side forward matched closely the peak in counterfield rotation, while the minima in propulsion velocity matched the transition frequency from counterfield to cofield rotation. Furthermore, based on electroorientation measurements for prolate Janus ellipsoids, we conclude that the propulsion velocity of spherical Janus particles reflects the real part of their polarizability. Solutions of the Poisson-Nernst-Planck equations confirm the thickness of the metal cap facilitates adjusting the behavior from metal- to dielectric-like. These traits translate into different collective behaviors, such as the ability to traverse or become part of a lattice of nonpatchy silica particles. Overall, these results provide experimental evidence to either challenge or refine existing electrokinetic models of propulsion.

Electro-Orientation and Electro-Rotation of Metallodielectric Janus Particles.

The electro-rotation (EROT) and electro-orientation (EOR) behavior of metallodielectric spherical Janus particles (JP) are studied analytically and verified experimentally. This stands in contrast to previous either heuristic or numerically computed models of JP dipoles. First, we obtain frequency-dependent analytic expressions for the corresponding dipole terms for a JP composed of dielectric and metallic hemispheres by applying the "standard" (weak-field) electrokinetic model and using a Fourier-Legendre collocation method for solving two sets of linear equations. EROT and EOR spectra, describing the variation of the JP's angular velocity on the forcing frequency of a rotating and nonrotating spatially uniform electric field, respectively, are explicitly determined and compared against experiments (different JP sizes and solution conductivities). While a favorably good agreement between theory and experimental measurements was found for the frequency response (∼8% difference), there is still a factor of ∼2 difference in the amplitude of the angular velocity, which necessitates further future improvements to the model.

Collective diffusion in a two-dimensional liquid composed of Janus particles

The collective diffusion of anisotropic particles in liquids plays a crucial role in many processes, such as self-assembly. The patchy particle, which is usually nearly spherical in shape, is an important anisotropic particle with different properties from other anisotropic particles like the ellipsoid liquid crystal particles. In the present study, molecular dynamics simulations are performed to study the collective diffusion of a two-dimensional anisotropic liquid system composed of Janus particles. The static structures and diffusion behaviours of anisotropic and isotropic Lennard-Jones liquids are compared. The long-time diffusion behaviour of an anisotropic liquid of nearly spherical Janus particles is found to be similar to that of an isotropic liquid because the orientation of the particles disappears over long-term averaging. The anisotropic properties of the Janus particles are mainly reflected in the spatial correlation of particle orientations and mid-time diffusion behaviour. The difference between nearly spherical anisotropic particles and rod-like particles is also discussed in this paper.

Self-thermophoresis of laser-heated spherical Janus particles

An analytic framework is presented for calculating the self-induced thermophoretic velocity of a laser-heated Janus metamaterial micro-particle, consisting of two conducting hemispheres of different thermal and electric conductivities. The spherical Janus is embedded in a quiescent fluid of infinite expanse and is exposed to a continuous light irradiation by a defocused laser beam. The analysis is carried under the electrostatic (Rayleigh) approximation (radius small compared to wavelength). The linear scheme for evaluating the temperature field in the three phases is based on employing a Fourier–Legendre approach, which renders rather simple semi-analytic expressions in terms of the relevant physical parameters of the titled symmetry-breaking problem. In addition to an explicit solution for the self-thermophoretic mobility of the heated Janus, we also provide analytic expressions for the slip-induced Joule heating streamlines and vorticity field in the surrounding fluid, for a non-uniform (surface dependent) Soret coefficient. For a ‘symmetric’ (homogeneous) spherical particle, the surface temperature gradient vanishes and thus there is no self-induced thermophoretic velocity field. The ‘inner’ temperature field in this case reduces to the well-known solution for a laser-heated spherical conducting colloid. In the case of a constant Soret phoretic mobility, the analysis is compared against numerical simulations, based on a tailored collocation method for some selected values of the physical parameters. Also presented are some typical temperature field contours and heat flux vectors prevailing in the two-phase Janus as well as light-induced velocity and vorticity fields in the ambient solute and a new practical estimate for the self-propelling velocity.Graphic abstract

Rational Design of Self-Propelling Particles for Unified Cargo Loading and Transportation.

Recent studies on electrically powered active particles that can both self-propel and manipulate cargo load and release, have focused on both spherically shaped Janus particles (JP) and on a parallel electrically conducting plates setup. Yet, spherically shaped JPs set a geometrical limitation on the ability to smartly design multiple dielectrophoretic traps on a single active particle. Herein, these active carriers are extended to accommodate any desired shape and selective metallic coating, using a standard photolithography method. The resulting designed positive and negative dielectrophoretic traps of controlled size, location, and intensity, performed as sophisticated active carriers with a high level of control over their mobility and cargo loading. In addition to cargo loading, the engineered particles exhibit interesting motion in an electrically insulating substrate setup, with in-plane electric field, and, in particular, a tilt angle, and even flipping, that strongly depended on the field frequency and amplitude, hence, exhibiting a much more diverse and rich behavior than spherical JP. The engineered self-propelling carriers are expected to open up new possibilities for unified, label-free and selective cargo loading, transport, and delivery of complex multi-particles.

AdaPT: Adaptable Particle Tracking for spherical microparticles in lab on chip systems

Due to its rising importance in science and technology in recent years, particle tracking in videos presents itself as a tool for successfully acquiring new knowledge in the field of life sciences and physics. Accordingly, different particle tracking methods for various scenarios have been developed. In this article, we present a particle tracking application implemented in Python for, in particular, spherical magnetic particles, including superparamagnetic beads and Janus particles. In the following, we distinguish between two sub-steps in particle tracking, namely the localization of particles in single images and the linking of the extracted particle positions of the subsequent frames into trajectories. We provide an intensity-based localization technique to detect particles and two linking algorithms, which apply either frame-by-frame linking or linear assignment problem solving. Beyond that, we offer helpful tools to preprocess images automatically as well as estimate parameters required for the localization algorithm by utilizing machine learning. As an extra, we have implemented a technique to estimate the current spatial orientation of Janus particles within the x–y-plane. Our framework is readily extendable and easy-to-use as we offer a graphical user interface and a command-line tool. Various output options, such as data frames and videos, ensure further analysis that can be automated. Program summaryProgram Title: AdaPTCPC Library link to program files:https://doi.org/10.17632/xxpnsbv3cs.1Developer’s repository link:https://git.ies.uni-kassel.de/adapt/adaptLicensing provisions: MPL-2.0Programming language: Python 3.6Supplementary material: We provide supplementary material to increase the traceability of the provided example. It consists of an exemplary input video, the corresponding annotated video with tracked particles, a data frame including the tracking information, and a plot displaying the trajectories.Nature of problem: Particle tracking in videos is an important tool for acquiring new knowledge in diverse fields. Several particle tracking methods have been developed for these diverse applications. The presented particle tracking software has been developed for the motion analysis of spherical or close to spherical magnetic particles. Up until now, no easily extensible automated particle tracking software for close to spherical microparticles and their current positioning status is available.Solution method: AdaPT is an extensible, easy-to-use microparticle tracking application developed explicitly for lab on chip applications but easily extensible to other applications and further functionalities. Currently implemented linking algorithms are a frame-by-frame linking approach as well as an approach solving linear assignment problems. In addition to many assistance possibilities for the user in the form of estimates of parameter values through machine learning, we offer the particular option to determine the orientation and rotation of spherical polymer particles with hemispherical metallic caps (Janus particles). The application can be used via console and graphical user interface.Additional comments including restrictions and unusual features: This software requires video data with spherical or close to spherical magnetic particles. It was tested on videos containing spherical superparamagnetic and magnetic Janus particles. Only mobile particles are detected; immobile particles are ignored by the software, reducing the amount of output data considerably. As a unique feature, the spatial orientation within the x–y-plane of Janus particles can be determined. The application has been tested on a variety of two-dimensional particle motion patterns. The latest version of AdaPT can be found here: https://git.ies.uni-kassel.de/adapt/adapt.

Controlling Janus Nanodisc Topology through ABC Triblock Terpolymer/Homopolymer Blending in 3D Confinement

Janus particles have drawn considerable interest as colloidal surfactants, microswimmers, and building blocks for colloidal lattices. So far, research primarily focused on spherical Janus particles for which a number of fabrication methods are well established. Janus particles with geometric anisotropy offer shape-dependent properties in addition to surface anisotropy, but their synthesis is more challenging. Here, we report a variety of polymeric Janus nanoparticles synthesized from ABC triblock terpolymer microphases in microemulsion droplets. Evaporation-induced assembly of the ABC triblock terpolymers led to prolate microparticles with A/C lamellae stacked along the particle’s major axis. By admixing a B homopolymer during microphase separation, the morphology of the B microphase was gradually tuned in between the A/C lamellae. Cross-linking of the B microdomain created Janus nanodiscs, where the topology could be controlled to unconventional inner structures. We follow the morphology evolution and rationalize their stability with theoretical considerations in the strong segregation limit and dissipative particle dynamics simulations.

Substrate wettability guided oriented self assembly of Janus particles

Self-assembly of Janus particles with spatial inhomogeneous properties is of fundamental importance in diverse areas of sciences and has been extensively observed as a favorably functionalized fluidic interface or in a dilute solution. Interestingly, the unique and non-trivial role of surface wettability on oriented self-assembly of Janus particles has remained largely unexplored. Here, the exclusive role of substrate wettability in directing the orientation of amphiphilic metal-polymer Bifacial spherical Janus particles, obtained by topo-selective metal deposition on colloidal Polymestyere (PS) particles, is explored by drop casting a dilute dispersion of the Janus colloids. While all particles orient with their polymeric (hydrophobic) and metallic (hydrophilic) sides facing upwards on hydrophilic and hydrophobic substrates respectively, they exhibit random orientation on a neutral substrate. The substrate wettability guided orientation of the Janus particles is captured using molecular dynamic simulation, which highlights that the arrangement of water molecules and their local densities near the substrate guide the specific orientation. Finally, it is shown that by spin coating it becomes possible to create a hexagonal close-packed array of the Janus colloids with specific orientation on differential wettability substrates. The results reported here open up new possibilities of substrate-wettability driven functional coatings of Janus particles, which has hitherto remained unexplored.

Preparation of Cylindrical Janus Particles Using a Stirring Method.

We previously discovered a novel method for the preparation of polymer particles that have a cylindrical shape. Polystyrene (PS) or poly methyl methacrylate (PMMA) spherical particles were deformed into a cylindrical shape by stirring with a magnetic stirrer in a polyvinylpyrrolidone (PVP) aqueous solution. In this study, cylindrical “Janus” particles consisting of PS and PMMA were prepared by this stirring method. In the case of spherical Janus particles, cylindrical particles were obtained after stirring; however, the direction of the interface between the PS and PMMA phases was random. However, in the case of snowman-like Janus particles, cylindrical Janus particles with the interface at the center of the long axis were successfully prepared. This indicated that the extension direction can be controlled owing to the anisotropic shape and supported the proposed deformation mechanism of the cylindrical particles. Moreover, amphiphilic cylindrical Janus particles were also successfully prepared by hydrolysis of only one phase to introduce carboxy groups.

Dielectrophoretic Force Equilibrium of Complex Particles

In contrast to the commonly used spherical Janus particles, here we used engineered Janus particles that are fabricated using photolithography technique for precise control over their geometry and coated regions. Specifically, we studied a lollipop-shaped complex particle where its head is coated with gold while its tail is left bare. Due to their distinct electrical properties (i.e. electrical polarizability) the particle exhibits force equilibrium where opposite dielectrophoretic forces acting on its head and tail exactly cancel each other to yield a stable equilibrium position. This was realized in a quadrupolar electrode array where the equilibrium position of the engineered particle could be tuned by the frequency. This stands in contrast to the standard dielectrophoretic behavior where the particle shifts positions from either the center of the quad to the very edge of the electrodes when shifting from a negative to positive dielectrophoretic response, respectively. This opens new opportunities for positioning control of such complex particles for self-assembly, biosensing, biomimetic spermatozoa and more.

Self-propelled torus colloids.

Suspensions of chemically powered self-propelled colloidal particles are examples of active matter systems with interesting properties. While simple spherical Janus particles are often studied, it is known that geometry is important and recent experiments have shown that chemically active torus-shaped colloids behave differently from spherical colloids. In this paper, coarse-grained microscopic simulations of the dynamics of self-diffusiophoretic torus colloids are carried out in bulk solution in order to study how torus geometric factors influence their active motion. The concentration and velocity fields are key ingredients in self-diffusiophoretic propulsion, and the forms that these fields take in the colloid vicinity are shown to be strong functions of torus geometric parameters such as the torus hole size and thickness of the torus tube. This work utilizes a method where self-diffusiophoretic torus colloids with various geometric and dynamical characteristics can be built and studied in fluid media that include chemical reactions and fluid flows. The model can be used to investigate the collective properties of these colloids and their dynamics in confined systems, topics that are of general importance for applications that use colloidal motors with complex geometries.

Reactive Momentum Transfer Contributes to the Self-Propulsion of Janus Particles.

We report simulations of a spherical Janus particle undergoing exothermic surface reactions around one pole only. Our model excludes self-phoretic transport by design. Nevertheless, net motion occurs from direct momentum transfer between solvent and colloid, with speed scaling as the square root of the energy released during the reaction. We find that such propulsion is dominated by the system's short-time response, when neither the time dependence of the flow around the colloid nor the solvent compressibility can be ignored. Our simulations agree reasonably well with previous experiments.

Measurement of the capillary interaction force between Janus colloidal particles trapped at a flat air/water interface

The capillary interaction force between spherical Janus particles trapped at the air-water interface is measured using a time-sharing optical tweezer (bond number ≪ 1). One face of the particles is hydrophilic, and the other one, hydrophobic. Measured force goes from almost pure quadrupolar to almost pure hexapolar interaction due to the three-phase contact line corrugation. Measured force curves are modeled as a sum of power laws, Ar-α + Br-β + Cr-γ, obtained from an expansion in capillary multipoles. The mean values for the exponents of particle pairs of 3 μm are α = 5.05 ± 0.12, β = 7.02 ± 0.03, and γ = 5.96 ± 0.03. For particles pairs of 5 μm, we find α = 5.02 ± 0.04, β = 6.94 ± 0.06, and γ = 5.80 ± 0.05. In both cases, A < 0, B < 0, and C > 0.

Direct numerical simulation of the self-propelled Janus particle: use of grid-refined fluctuating lattice Boltzmann method

The study of the microscopic propelling mechanism of anisotropic Janus particles often involves the analysis of motion at multi-time scale. In this paper, an efficient method is developed for directly simulating the motion of non-equilibrium particles to resolve the issue of requiring large computational resources to simulate the complex multi-time scale motion of Janus particles. We combined fluctuating lattice Boltzmann method and grid-refinement technology to simulate spherical and cylindrical Janus particles, and compared their motion characteristics with experimental results at multi-time scales, which proved that the method is efficient and feasible. This simulation method can also be applied to more complex active particle motion systems.

On the Elastic Description of a Spherical Janus Particle

Abstract The elastic problem of a spherical core-shell particle with a truncated core is solved within the isotropic classical theory of elasticity. A transition to a Janus particle consisting of two unequal spherical segments with lattice mismatch is demonstrated. Elastic fields in the Janus particle are found and described in detail. The strain energy of the Janus particle in dependence on the interface coordinate is discussed.

A Pickering Emulsion Route to Swimming Active Janus Colloids.

The field of active colloids is attracting significant interest to both enable applications and allow investigations of new collective colloidal phenomena. One convenient active colloidal system that has been much studied is spherical Janus particles, where a hemispherical coating of platinum decomposes hydrogen peroxide to produce rapid motion. However, at present producing these active colloids relies on a physical vapor deposition (PVD) process, which is difficult to scale and requires access to expensive equipment. In this work, it is demonstrated that Pickering emulsion masking combined with solution phase metallization can produce self‐motile catalytic Janus particles. Comparison of the motion and catalytic activity with PVD colloids reveals a higher catalytic activity for a given thickness of platinum due to the particulate nature of the deposited coating. This Pickering emulsion based method will assist in producing active colloids for future applications and aid experimental research into a wide range of active colloid phenomena.