Densitaxis: Active particle motion in density gradients.

Organisms often swim through density-stratified fluids. Here, we investigate the dynamics of active particles swimming in fluid density gradients and report theoretical evidence of taxis as a result of these gradients (densitaxis). Specifically, we calculate the effect of density stratification on the dynamics of a force- and torque-free spherical squirmer and show that density gradients induce reorientation that tends to align swimming either parallel or normal to the gradient depending on the swimming gait. In particular, swimmers that propel by generating thrust in the front (pullers) rotate to swim parallel to gradients and hence display (positive or negative) densitaxis, while swimmers that propel by generating thrust in the back (pushers) rotate to swim normal to the gradients. This work could be useful to understand the motion of marine organisms in ocean or be leveraged to sort or organize a suspension of active particles by modulating density gradients.

Self-propelling colloids with finite state dynamics.

Endowing materials with the ability to sense, adapt, and respond to stimuli holds the key to a progress leap in autonomous systems. In spite of the growing success of macroscopic soft robotic devices, transferring these concepts to the microscale presents several challenges connected to the lack of suitable fabrication and design techniques and of internal response schemes that connect the materials' properties to the function of the active units. Here, we realize self-propelling colloidal clusters which possess a finite number of internal states, which define their motility and which are connected by reversible transitions. We produce these units via capillary assembly combining hard polystyrene colloids with two different types of thermoresponsive microgels. The clusters, actuated by spatially uniform AC electric fields, adapt their shape and dielectric properties, and consequently their propulsion, via reversible temperature-induced transitions controlled by light. The different transition temperatures for the two microgels enable three distinct dynamical states corresponding to three illumination intensity levels. The sequential reconfiguration of the microgels affects the velocity and shape of the active trajectories according to a pathway defined by tailoring the clusters' geometry during assembly. The demonstration of these simple systems indicates an exciting route toward building more complex units with broader reconfiguration schemes and multiple responses as a step forward in the pursuit of adaptive autonomous systems at the colloidal scale.

Robust acoustic trapping and perturbation of single-cell microswimmers illuminate three-dimensional swimming and ciliary coordination.

We report a label-free acoustic microfluidic method to confine single, cilia-driven swimming cells in space without limiting their rotational degrees of freedom. Our platform integrates a surface acoustic wave (SAW) actuator and bulk acoustic wave (BAW) trapping array to enable multiplexed analysis with high spatial resolution and trapping forces that are strong enough to hold individual microswimmers. The hybrid BAW/SAW acoustic tweezers employ high-efficiency mode conversion to achieve submicron image resolution while compensating for parasitic system losses to immersion oil in contact with the microfluidic chip. We use the platform to quantify cilia and cell body motion for wildtype biciliate cells, investigating effects of environmental variables like temperature and viscosity on ciliary beating, synchronization, and three-dimensional helical swimming. We confirm and expand upon the existing understanding of these phenomena, for example determining that increasing viscosity promotes asynchronous beating. Motile cilia are subcellular organelles that propel microorganisms or direct fluid and particulate flow. Thus, cilia are critical to cell survival and human health. The unicellular alga Chlamydomonas reinhardtii is widely used to investigate the mechanisms underlying ciliary beating and coordination. However, freely swimming cells are difficult to image with sufficient resolution to capture cilia motion, necessitating that the cell body be held during experiments. Acoustic confinement is a compelling alternative to use of a micropipette, or to magnetic, electrical, and optical trapping that may modify the cells and affect their behavior. Beyond establishing our approach to studying microswimmers, we demonstrate a unique ability to mechanically perturb cells via rapid acoustic positioning.

Fatal attraction: How Phytophthora zoospores find their host.

Oomycete plant pathogens, such as Phytophthora and Pythium species produce motile dispersal agents called zoospores that actively target host plants. Zoospores are exceptional in their ability to display taxis to chemical, electrical and physical cues to navigate the phyllosphere and reach stomata, wound sites and roots. Many components of root exudates have been shown attractive or repulsive to zoospores. Although some components possess very strong attractiveness, it seems that especially the mix of components exuded by the primary host is most attractive to zoospores. Zoospores actively approach attractants with swimming behaviour reminiscent of other microswimmers. To achieve a unified description of zoospore behaviour when sensing an attractant, we propose the following terms for the successive stages of the homing response: reorientation, approaching, retention and settling. How zoospores sense and process attractants is poorly understood but likely involves signal perception via cell surface receptors. Since zoospores are important for infection, undermining their activity by luring attractants or blocking receptors seem promising strategies for disease control.

Chemotactic self-caging in active emulsions.

A common feature of biological self-organization is how active agents communicate with each other or their environment via chemical signaling. Such communications, mediated by self-generated chemical gradients, have consequences for both individual motility strategies and collective migration patterns. Here, in a purely physicochemical system, we use self-propelling droplets as a model for chemically active particles that modify their environment by leaving chemical footprints, which act as chemorepulsive signals to other droplets. We analyze this communication mechanism quantitatively both on the scale of individual agent-trail collisions as well as on the collective scale where droplets actively remodel their environment while adapting their dynamics to that evolving chemical landscape. We show in experiment and simulation how these interactions cause a transient dynamical arrest in active emulsions where swimmers are caged between each other's trails of secreted chemicals. Our findings provide insight into the collective dynamics of chemically active particles and yield principles for predicting how negative autochemotaxis shapes their navigation strategy.

Hopping trajectories due to long-range interactions determine surface accumulation of microalgae.

The accumulation of motile cells at solid interfaces increases the rate of surface encounters and the likelihood of surface attachment, leading to surface colonization and biofilm formation. The cell density distribution in the vicinity of a physical boundary is influenced by the interactions between the microswimmers and their physical environment, including hydrodynamic and steric interactions, as well as by stochastic effects. Disentangling the contributions of these effects remains an experimental challenge. Here, we use a custom-made four-camera view microscope to track a population of motile puller-type Chlamydomonas reinhardtii in a relatively unconstrained three-dimensional (3D) domain. Our experiments yield an extensive sample of 3D trajectories including cell-surface encounters with a planar wall, from which we extract a full description of the dynamics and the stochasticity of swimming cells. We use this large data sample and combine it with Monte Carlo simulations to determine the link between the dynamics at the single-cell level and the cell density. Our experiments demonstrate that the near-wall scattering is bimodal, corresponding to steric and hydrodynamic effects. We find, however, that this near-wall dynamics has little influence on the cell accumulation at the surface. On the other hand, we present evidence of a cell-induced surface-directed rotation leading to a vertical orbiting behavior and hopping trajectories, consistent with long-range hydrodynamic effects. We identify this long-range effect to be at the origin of the significant surface accumulation of cells.

Emergent probability fluxes in confined microbial navigation.

When the motion of a motile cell is observed closely, it appears erratic, and yet the combination of nonequilibrium forces and surfaces can produce striking examples of organization in microbial systems. While most of our current understanding is based on bulk systems or idealized geometries, it remains elusive how and at which length scale self-organization emerges in complex geometries. Here, using experiments and analytical and numerical calculations, we study the motion of motile cells under controlled microfluidic conditions and demonstrate that probability flux loops organize active motion, even at the level of a single cell exploring an isolated compartment of nontrivial geometry. By accounting for the interplay of activity and interfacial forces, we find that the boundary's curvature determines the nonequilibrium probability fluxes of the motion. We theoretically predict a universal relation between fluxes and global geometric properties that is directly confirmed by experiments. Our findings open the possibility to decipher the most probable trajectories of motile cells and may enable the design of geometries guiding their time-averaged motion.

Hyper-Ballistic Superdiffusion of Competing Microswimmers.

Hyper-ballistic diffusion is shown to arise from a simple model of microswimmers moving through a porous media while competing for resources. By using a mean-field model where swimmers interact through the local concentration, we show that a non-linear Fokker-Planck equation arises. The solution exhibits hyper-ballistic superdiffusive motion, with a diffusion exponent of four. A microscopic simulation strategy is proposed, which shows excellent agreement with theoretical analysis.

Molecular Imprinted BiVO4 Microswimmers for Selective Target Recognition and Removal.

Analogous to photosynthetic systems, photoactive semiconductor-based micro/nanoswimmers display biomimetic features that enable unique light harvesting and energy conversion functions and interactions with their surroundings. However, these artificial swimmers are usually non-selective and provide ineffective target recognition, resulting in poor surface analyte binding that affects the overall reactivity and motion efficiency. Here, the surface engineering of light-driven BiVO4 microswimmers by molecular imprinting polymerization is presented. After embedding surface recognition sites, the modified microswimmers can self-propel in a solution of a target molecule, without requiring toxic fuels, and degrade the target selectively in a pollutant mixture. These findings show that optimizing the design of semiconductor-based microswimmers with specific target recognition cavities on their surface is a promising strategy to achieve selective capture and degradation of organic pollutants, which is otherwise impossible because of the non-selective behavior of photogenerated reactive radicals. Moreover, this study provides a unique strategy to enhance the motion capabilities of single-component photocatalytic microswimmers in a specific chemical environment.

Acoustically powered surface-slipping mobile microrobots.

Untethered synthetic microrobots have significant potential to revolutionize minimally invasive medical interventions in the future. However, their relatively slow speed and low controllability near surfaces typically are some of the barriers standing in the way of their medical applications. Here, we introduce acoustically powered microrobots with a fast, unidirectional surface-slipping locomotion on both flat and curved surfaces. The proposed three-dimensionally printed, bullet-shaped microrobot contains a spherical air bubble trapped inside its internal body cavity, where the bubble is resonated using acoustic waves. The net fluidic flow due to the bubble oscillation orients the microrobot's axisymmetric axis perpendicular to the wall and then propels it laterally at very high speeds (up to 90 body lengths per second with a body length of 25 µm) while inducing an attractive force toward the wall. To achieve unidirectional locomotion, a small fin is added to the microrobot's cylindrical body surface, which biases the propulsion direction. For motion direction control, the microrobots are coated anisotropically with a soft magnetic nanofilm layer, allowing steering under a uniform magnetic field. Finally, surface locomotion capability of the microrobots is demonstrated inside a three-dimensional circular cross-sectional microchannel under acoustic actuation. Overall, the combination of acoustic powering and magnetic steering can be effectively utilized to actuate and navigate these microrobots in confined and hard-to-reach body location areas in a minimally invasive fashion.

Carbon nitride-based light-driven microswimmers with intrinsic photocharging ability.

Controlling autonomous propulsion of microswimmers is essential for targeted drug delivery and applications of micro/nanomachines in environmental remediation and beyond. Herein, we report two-dimensional (2D) carbon nitride-based Janus particles as highly efficient, light-driven microswimmers in aqueous media. Due to the superior photocatalytic properties of poly(heptazine imide) (PHI), the microswimmers are activated by both visible and ultraviolet (UV) light in conjunction with different capping materials (Au, Pt, and SiO2) and fuels (H2O2 and alcohols). Assisted by photoelectrochemical analysis of the PHI surface photoreactions, we elucidate the dominantly diffusiophoretic propulsion mechanism and establish the oxygen reduction reaction (ORR) as the major surface reaction in ambient conditions on metal-capped PHI and even with TiO2-based systems, rather than the hydrogen evolution reaction (HER), which is generally invoked as the source of propulsion under ambient conditions with alcohols as fuels. Making use of the intrinsic solar energy storage ability of PHI, we establish the concept of photocapacitive Janus microswimmers that can be charged by solar energy, thus enabling persistent light-induced propulsion even in the absence of illumination-a process we call "solar battery swimming"-lasting half an hour and possibly beyond. We anticipate that this propulsion scheme significantly extends the capabilities in targeted cargo/drug delivery, environmental remediation, and other potential applications of micro/nanomachines, where the use of versatile earth-abundant materials is a key prerequisite.

Diffusion-Limited Processes in Hydrogels with Chosen Applications from Drug Delivery to Electronic Components.

Diffusion is one of the key nature processes which plays an important role in respiration, digestion, and nutrient transport in cells. In this regard, the present article aims to review various diffusion approaches used to fabricate different functional materials based on hydrogels, unique examples of materials that control diffusion. They have found applications in fields such as drug encapsulation and delivery, nutrient delivery in agriculture, developing materials for regenerative medicine, and creating stimuli-responsive materials in soft robotics and microrobotics. In addition, mechanisms of release and drug diffusion kinetics as key tools for material design are discussed.

Hybrid Enzymatic/Photocatalytic Degradation of Antibiotics via Morphologically Programmable Light-Driven ZnO Microrobots.

Antibiotics are antimicrobial substances that can be used for preventive and therapeutic purposes in humans and animals. Their overdose usage has led to uncontrolled release to the environment, contributing significantly to the development of antimicrobial resistance phenomena. Here, enzyme-immobilized self-propelled zinc oxide (ZnO) microrobots are proposed to effectively target and degrade the released antibiotics in water bodies. Specifically, the morphology of the microrobots is tailored via the incorporation of Au during the synthetic process to lead the light-controlled motion into having on/off switching abilities. The microrobots are further modified with laccase enzyme by physical adsorption, and the immobilization process is confirmed by enzymatic activity measurements. Oxytetracycline (OTC) is used as a model of veterinary antibiotics to investigate the enzyme-immobilized microrobots for their removal capacities. The results demonstrate that the presence of laccase on the microrobot surfaces can enhance the removal of antibiotics via oxidation. This concept for immobilizing enzymes on self-propelled light-driven microrobots leads to the effective removal of the released antibiotics from water bodies with an environmentally friendly strategy.

CeFlowBot: A Biomimetic Flow-Driven Microrobot that Navigates under Magneto-Acoustic Fields.

Aquatic organisms within the Cephalopoda family (e.g., octopuses, squids, cuttlefish) exist that draw the surrounding fluid inside their bodies and expel it in a single jet thrust to swim forward. Like cephalopods, several acoustically powered microsystems share a similar process of fluid expulsion which makes them useful as microfluidic pumps in lab-on-a-chip devices. Herein, an array of acoustically resonant bubbles are employed to mimic this pumping phenomenon inside an untethered microrobot called CeFlowBot. CeFlowBot contains an array of vibrating bubbles that pump fluid through its inner body thereby boosting its propulsion. CeFlowBots are later functionalized with magnetic layers and steered under combined influence of magnetic and acoustic fields. Moreover, acoustic power modulation of CeFlowBots is used to grasp nearby objects and release it in the surrounding workspace. The ability of CeFlowBots to navigate remote environments under magneto-acoustic fields and perform targeted manipulation makes such microrobots useful for clinical applications such as targeted drug delivery. Lastly, an ultrasound imaging system is employed to visualize the motion of CeFlowBots which provides means to deploy such microrobots in hard-to-reach environments inaccessible to optical cameras.

Fabrication of magnetic helical microribbons made of nickel thin films sandwiched between silicon nitride layers for microswimming applications.

Helical swimming is adopted by microswimming robots since it is an efficient mechanism and commonly observed among microorganisms swimming at low Reynolds numbers. However, manufacturing of micro-helices made of sub-micron magnetic thin layers is neither straightforward nor well-established, advanced materials and methods are necessary to obtain such structures as reported in the literature. In this paper, a topological patterning method utilizing basic microfabrication methods is presented for the self-assembly of magnetic micro-helices made of a sandwiched nickel thin film (50-150 nm) between two silicon nitride layers. Strain mismatch between the thin films and the geometric anisotropy introduced by the slanted patterns on the top nitride layer result in self-rolled-up helical microribbons. Moreover, inspired by the actual release process during the wet-etching of the microribbon from the substrate, moving boundary conditions are incorporated in a numerical model to simulate the self-rolling of trilayer ribbons. The simulation results are compared and validated by experimental data within 7% error for all cases, including the geometries that do not result in a helical shape. The swimming performance of the magnetized micro-helix is demonstrated inside a capillary glass tube experimentally and cross-validated with a numerical model.

Spatially Controlled CO2 Conversion Kinetics in Natural Leaves for Motion Generation.

Living systems that can spontaneously exhibit directional motion belong to diverse classes such as bacteria, sperm and plankton. They have fascinated scientists in recent years to design completely artificial or biohybrid mobile objects. Natural ingredients, like parts of plants, have been used to elaborate miniaturized dynamic objects, which can move when they are combined with other, non-natural, building blocks. Herein, we report that the precise structural tailoring of natural plant leaves allows generating a spatially predefined and confined release of oxygen gas, due to the conversion of carbon dioxide. This constitutes the driving force for generating motion, which is solely due to the respiration of leaves by photosynthesis. The rate of gas evolution can be fine-tuned by changing the light intensity and the leaf size, allowing ultimately to control the motility of objects with dimensions ranging from the millimeter to the micrometer scale.

Autonomous Chiral Microswimmers with Self-mixing Capabilities for Highly Efficient Enantioselective Synthesis.

The development of chiral catalysts plays a very important role in various areas of chemical science. Heterogeneous catalysts have the general advantage of allowing a more straightforward separation from the products. One specific case of heterogeneous catalysis is electrocatalysis, being potentially a green chemistry approach. However, a typical drawback is that the redox conversion of molecules occurs only at the electrode/electrolyte interface, and not in the bulk of the electrolyte. The second limitation is that the electrodes have to be physically connected to a power supply to induce the desired reactions. To circumvent these problems, we propose here a complementary approach by replacing macroscopic electrodes with an ensemble of self-propelled redox active microswimmers. They move autonomously in solution while transforming simultaneously a prochiral starting compound into a specific enantiomer with a very high enantiomeric excess, accompanied by a significantly increased production rate of the favorite enantiomer.

Microfluidics for Microswimmers: Engineering Novel Swimmers and Constructing Swimming Lanes on the Microscale, a Tutorial Review.

This paper provides an updated review of recent advances in microfluidics applied to artificial and biohybrid microswimmers. Sharing the common regime of low Reynolds number, the two fields have been brought together to take advantage of the fluid characteristics at the microscale, benefitting microswimmer research multifold. First, microfluidics offer simple and relatively low-cost devices for high-fidelity production of microswimmers made of organic and inorganic materials in a variety of shapes and sizes. Microscale confinement and the corresponding fluid properties have demonstrated differential microswimmer behaviors in microchannels or in the presence of various types of physical or chemical stimuli. Custom environments to study these behaviors have been designed in large part with the help of microfluidics. Evaluating microswimmers in increasingly complex lab environments such as microfluidic systems can ensure more effective implementation for in-field applications. The benefits of microfluidics for the fabrication and evaluation of microswimmers are balanced by the potential use of microswimmers for sample manipulation and processing in microfluidic systems, a large obstacle in diagnostic and other testing platforms. In this review various ways in which these two complementary technology fields will enhance microswimmer development and implementation in various fields are introduced.

Cooperative Chemotaxis of Magnesium Microswimmers for Corrosion Spotting.

Numerous artificial micro- and nanomotors, as well as various swimmers have been inspired by living organisms that are able to move in a coordinated manner. Their cooperation has also gained a lot of attention because the resulting clusters are able to adapt to changes in their environment and to perform complex tasks. However, mimicking such a collective behavior remains a challenge. In the present work, magnesium microparticles are used as chemotactic swimmers with pronounced collective features, allowing the gradual formation of macroscopic agglomerates. The formed clusters act like a single swimmer able to follow pH gradients. This dynamic behavior can be used to spot localized corrosion events in a straightforward way. The autonomous docking of the swimmers to the corrosion site leads to the formation of a local protection layer, thus increasing corrosion resistance and triggering partial self-healing.

Confined Bubble-Propelled Microswimmers in Capillaries: Wall Effect, Fuel Deprivation, and Exhaust Product Excess.

Self-propelled autonomous nano/microswimmers are at the forefront of materials science. These swimmers are expected to operate in highly confined environments, such as between the grains of soil or in the capillaries of the human organism. To date, little attention is paid to the problem that in such a confined environment the fuel powering catalytic nano/microswimmers can be exhausted quickly and the space can be polluted with the product of the catalytic reaction. In addition, the motion of the nano/microswimmers may be influenced by the confinement. These issues are addressed here, showing the influence of the size of the capillary and length of the micromotor on the motion and the influence of the depletion of the fuel and excess of the exhaust products. Theoretical modeling is provided as well to bring further insight into the observations. This article shows challenges that these systems face and stimulates research to overcome them.