Phoresis kernel theory for passive and active spheres with nonuniform phoretic mobility.

By introducing geometry-based phoresis kernels, we establish a direct connection between the translational and rotational velocities of a phoretic sphere and the distributions of the driving fields or fluxes. The kernels quantify the local contribution of the field or flux to the particle dynamics. The field kernels for both passive and active particles share the same functional form, depending on the position-dependent surface phoretic mobility. For uniform phoretic mobility, the translational field kernel is proportional to the surface normal vector, while the rotational field kernel is zero; thus, a phoretic sphere with uniform phoretic mobility does not rotate. As case studies, we discuss examples of a self-phoretic axisymmetric particle influenced by a globally-driven field gradient, a general scenario for axisymmetric self-phoretic particle and two of its special cases, and a non-axisymmetric active particle.

Smart Materials for Microrobots.

Over the past 15 years, the field of microrobotics has exploded with many research groups from around the globe contributing to numerous innovations that have led to exciting new capabilities and important applications, ranging from in vivo drug delivery, to intracellular biosensing, environmental remediation, and nanoscale fabrication. Smart responsive materials have had a profound impact on the field of microrobotics and have imparted small-scale robots with new functionalities and distinct capabilities. We have identified four large categories where the majority of future efforts must be allocated to push the frontiers of microrobots and where smart materials can have a major impact on such future advances. These four areas are the propulsion and biocompatibility of microrobots, the cooperation between individual units and human operators, and finally, the intelligence of microrobots. In this Review, we look critically at the latest developments in these four categories and discuss how smart materials contribute to the progress in the exciting field of microrobotics and will set the stage for the next generation of intelligent and programmable microrobots.

Nonstoichiometric Salt Intercalation as a Means to Stabilize Alkali Doping of 2D Materials.

Although doping with alkali atoms is a powerful technique for introducing charge carriers into physical systems, the resulting charge-transfer systems are generally not air stable. Here we describe computationally a strategy towards increasing the stability of alkali-doped materials that employs stoichiometrically unbalanced salt crystals with excess cations (which could be deposited during, e.g., in situ gating) to achieve doping levels similar to those attained by pure alkali metal doping. The crystalline interior of the salt crystal acts as a template to stabilize the excess dopant atoms against oxidation and deintercalation, which otherwise would be highly favorable. We characterize this doping method for graphene, NbSe_{2}, and Bi_{2}Se_{3} and its effect on direct-to-indirect band gap transitions, 2D superconductivity, and thermoelectric performance. Salt intercalation should be generally applicable to systems which can accommodate this "ionic crystal" doping (and particularly favorable when geometrical packing constraints favor nonstoichiometry).

Swimmers Heal on the Move Following Catastrophic Damage.

Herein, we describe the development of 2D self-healing small-scale swimmers capable of autonomous propulsion and "on-the-fly" structural recovery in large containers. Incorporation of magnetic Nd2Fe14B microparticles in specialized printed strips results in rapid reorientation and reattachment of the moving tail to its complementary broken static piece to restore the original swimmer structure and propulsion behavior. The swimmers display functional recovery independent of user input. Measurements of the magnetic hysteresis and fields were used to assess the behavior of the healing mechanism in real swimming situations. Damage position and multiple magnetic strip patterns have been examined and their influence upon the recovery efficiency has been compared. Owing to its versatility, fast response, and simplicity the new self-healing strategy represents an important step toward the development of new "on-the-fly" repairing strategies for small-scale swimmers and robots.

Geometrical Performance of Self-Phoretic Colloids and Microswimmers.

Within a unified formulation-encompassing self-electrophoresis, self-diffusiophoresis, and self-thermophoresis-we provide a simple integral kernel transforming the relevant surface flux to particle velocity for any spheroid with axisymmetric surface activity and uniform phoretic mobility. Appropriate scaling of the speed allows a dimensionless measure of the motion-producing performance of the motor shape and activity distribution across the surface. For bipartite designs with piecewise uniform flux over complementary surface regions, the performance is mapped out over the entire range of geometry (from discotic through spherical to rodlike shapes) and of bipartitioning, and intermediate aspect ratios that maximize performance are identified. Comparisons are made to experimental data from the literature.

Guiding chiral self-propellers in a periodic potential.

Ingenious suggestions continue to be made for separation of racemic mixtures according to the inert structural chirality of the constituents. Recently discovered self-motile micro- or nanoparticles express dynamical chirality, i.e., that which originates in motion, not structure. Here, we predict how dynamically chiral objects, with overdamped dynamics in a soft periodic two-dimensional potential, can display not only separation into well-defined dynamical subclasses defined by motility characteristics, but also the ability to be steered to arbitrary locations in the plane by simply changing the amplitude of the external potential. Orientational and translational diffusion produce new types of drift absent in the noise-free case. As practical implementation seems feasible with acoustic or optical fields, these phenomena can be useful for laboratory microscales manipulations, possibly including reconfigurable microfluidic circuits with complex networks of unidirectional channels.

Memory effects in spiral diffusion of rotary self-propellers.

The coupling of deterministic rotary motion and stochastic orientational diffusion of a self-propeller leads to a spiral trajectory of the expected displacement. We extend our former analysis of spiral diffusion [Phys. Rev. E 94, 030601(R) (2016)10.1103/PhysRevE.94.030601] in the white-noise limit to a more realistic scenario of stochastic noise with Gaussian memory and orientational fluctuations driven by an Ornstein-Uhlenbeck process. A variety of dynamical regimes including crossovers from ballistic to diffusive to ballistic in the angular dynamics are determined by the inertial timescale, orientational diffusivity, and angular speed.

Mutual information and breakdown of the Perron-Frobenius scenario in zero-temperature triangular Ising antiferromagnets on cylinders.

A nominally two-dimensional spin model wrapped onto a cylinder can profitably be viewed, especially for long cylinders, as a one-dimensional chain. Each site of such a chain is a ring of spins with a complex state space. Traditional correlation functions are inadequate for the study of correlations in such a system and need to be replaced with something like mutual information. Being induced purely by frustration, the disorder of a cylindrical zero-temperature triangular Ising antiferromagnet (TIAFM) and attendant correlations have a chance of evading the consequences of the Perron-Frobenius theorem which describes and constrains correlations in thermally disordered one-dimensional systems. Correlations in such TIAFM systems and the aforementioned evasion are studied here through a fermionic representation. For cylindrical TIAFM models with open boundary conditions, we explain and derive the following characteristics of end-to-end mutual information: period-three oscillation of the decay length, halving of the decay length compared to what Perron-Frobenius predicts on the basis of transfer matrix eigenvalues, and subexponential decay-inverse square in the length-for certain systems.

Modulating drift dynamics of circle swimmers by periodic potentials.

We propose a method to modulate the drifting motion of overdamped circle swimmers in steady fluid flows by means of static sinusoidal potentials. Using Langevin formalism, we study drift velocity as a function of potential strength and wavelength with and without diffusional motion. Drift velocity is essentially quantized without diffusion, but in the presence of noise, the displacement per cycle has a continuous range. As a function of dimensionless potential wave number, domains of damped oscillatory and plateau regimes are observed in the drift velocity diagram. At weak potential and fluid velocity less than powered velocity, there is also a regime where drift velocity exceeds the fluid velocity. Methods based on these results can be used to separate biological and artificial circle swimmers based on their dynamical properties.

Spontaneous directional flow of active magnetic particles.

We predict the emergence of large-scale polar order and spontaneous directional flows in a class of self-propelled autonomous particles that interact via passive repulsion between off-center sites. The coupling of active motion with the passive torque acting about the particle centers results in hybrid active-passive interactions responsible for a macroscopic phase transition from an isotropic state to a polar-aligned state in systems of particles with front interaction sites. We employ a continuum kinetic theory to explain that the emergence of long-ranged orientational order, which occurs in unbounded domains at finite densities, can be externally activated independently of the self-propulsion mechanism and drives a macroscopic particle flow in a direction selected by symmetry breaking.

Multigear Bubble Propulsion of Transient Micromotors.

Transient, chemically powered micromotors are promising biocompatible engines for microrobots. We propose a framework to investigate in detail the dynamics and the underlying mechanisms of bubble propulsion for transient chemically powered micromotors. Our observations on the variations of the micromotor active material and geometry over its lifetime, from initial activation to the final inactive state, indicate different bubble growth and ejection mechanisms that occur stochastically, resulting in time-varying micromotor velocity. We identify three processes of bubble growth and ejection, and in analogy with macroscopic multigear machines, we call each process a gear. Gear 1 refers to bubbles that grow on the micromotor surface before detachment while in Gear 2 bubbles hop out of the micromotor. Gear 3 is similar in nature to Gear 2, but the bubbles are too small to contribute to micromotor motion. We study the characteristics of these gears in terms of bubble size and ejection time, and how they contribute to micromotor displacement. The ability to tailor the shell polarity and hence the bubble growth and ejection and the surrounding fluid flow is demonstrated. Such understanding of the complex multigear bubble propulsion of transient chemical micromotors should guide their future design principles and serve for fine tuning the performance of these micromotors.

Built-In Active Microneedle Patch with Enhanced Autonomous Drug Delivery.

The use of microneedles has facilitated the painless localized delivery of drugs across the skin. However, their efficacy has been limited by slow diffusion of molecules and often requires external triggers. Herein, an autonomous and degradable, active microneedle delivery platform is introduced, employing magnesium microparticles loaded within the microneedle patch, as the built-in engine for deeper and faster intradermal payload delivery. The magnesium particles react with the interstitial fluid, leading to an explosive-like rapid production of H2 bubbles, providing the necessary force to breach dermal barriers and enhance payload delivery. The release kinetics of active microneedles is evaluated in vitro by measuring the amount of IgG antibody (as a model drug) that passed through phantom tissue and a pigskin barrier. In vivo experiments using a B16F10 mouse melanoma model demonstrate that the active delivery of anti-CTLA-4 (a checkpoint inhibitor drug) results in greatly enhanced immune response and significantly longer survival. Moreover, spatially resolved zones of active and passive microneedles allow a combinatorial rapid burst response along with slow, sustained release, respectively. Such versatile and effective autonomous dynamic microneedle delivery technology offers considerable promise for a wide range of therapeutic applications, toward a greatly enhanced outcome, convenience, and cost.

A Macrophage-Magnesium Hybrid Biomotor: Fabrication and Characterization.

Magnesium (Mg)-based micromotors are combined with live macrophage (MΦ) cells to create a unique MΦ-Mg biohybrid motor system. The resulting biomotors possess rapid propulsion ability stemming from the Mg micromotors and the biological functions provided by the live MΦ cell. To prepare the biohybrid motors, Mg microparticles coated with titanium dioxide and poly(l-lysine) (PLL) layers are incubated with live MΦs at low temperature. The formation of such biohybrid motors depends on the relative size of the MΦs and Mg particles, with the MΦ swallowing up Mg particles smaller than 5 µm. The experimental results and numerical simulations demonstrate that the motion of MΦ-Mg motors is determined by the size of the Mg micromotor core and the position of the MΦ during the attachment process. The MΦ-Mg motors also perform biological functions related to free MΦs such as endotoxin neutralization. Cell membrane staining and toxin neutralization studies confirm that the MΦs maintain their viability and functionality (e.g., endotoxin neutralization) after binding to the Mg micromotors. This new MΦ-Mg motor design can be expanded to different types of living cells to fulfill diverse biological tasks.

Engineering Contactless Particle-Particle Interactions in Active Microswimmers.

Artificial self-propelled colloidal particles have recently served as effective building blocks for investigating many dynamic behaviors exhibited by nonequilibrium systems. However, most studies have relied upon excluded volume interactions between the active particles. Experimental systems in which the mobile entities interact over long distances in a well-defined and controllable manner are valuable so that new modes of multiparticle dynamics can be studied systematically in the laboratory. Here, a system of self-propelled microscale Janus particles is engineered to have contactless particle-particle interactions that lead to long-range attraction, short-range repulsion, and mutual alignment between adjacent swimmers. The unique modes of motion that arise can be tuned by modulating the system's parameters.

Acoustic actuation of bioinspired microswimmers.

Acoustic actuation of bioinspired microswimmers is experimentally demonstrated. Microswimmers are fabricated in situ in a microchannel. Upon acoustic excitation, the flagellum of the microswimmer oscillates, which in turn generates linear or rotary movement depending on the swimmer design. The speed of these bioinspired microswimmers is tuned by adjusting the voltage amplitude applied to the acoustic transducer. Simple microfabrication and remote actuation are promising for biomedical applications.

Dynamic stabilization of Janus sphere trans-dimers.

We experimentally investigated the self-assembly of chemically active colloidal Janus spheres into dimers. The trans-dimer conformation, in which the two active sites are oriented roughly in opposite directions and the particles are osculated at their equators, becomes dominant as the hydrogen peroxide fuel concentration increases. Our observations suggest high spinning frequency combined with little translational motion is at least partially responsible for the stabilization of the trans-dimer as activity increases.

Spiral diffusion of rotating self-propellers with stochastic perturbation.

Translationally diffusive behavior arising from the combination of orientational diffusion and powered motion at microscopic scales is a known phenomenon, but the peculiarities of the evolution of expected position conditioned on initial position and orientation have been neglected. A theory is given of the spiral motion of the mean trajectory depending upon propulsion speed, angular velocity, orientational diffusion, and rate of random chirality reversal. We demonstrate the experimental accessibility of this effect using both tadpole-like and Janus sphere dimer rotating motors. Sensitivity of the mean trajectory to the kinematic parameters suggest that it may be a useful way to determine those parameters.

Acoustofluidic actuation of in situ fabricated microrotors.

We have demonstrated in situ fabricated and acoustically actuated microrotors. A polymeric microrotor with predefined oscillating sharp-edge structures is fabricated in situ by applying a patterned UV light to polymerize a photocrosslinkable polyethylene glycol solution inside a microchannel around a polydimethylsiloxane axle. To actuate the microrotors by oscillating the sharp-edge structures, we employed piezoelectric transducers which generate tunable acoustic waves. The resulting acoustic streaming flows rotate the microrotors. The rotation rate is tuned by controlling the peak-to-peak voltage applied to the transducer. A 6-arm microrotor can exceed 1200 revolutions per minute. Our technique is an integration of single-step microfabrication, instant assembly around the axle, and easy acoustic actuation for various applications in microfluidics and microelectromechanical systems (MEMS).

Self-consistent nonlocal feedback theory for electrocatalytic swimmers with heterogeneous surface chemical kinetics.

We present a self-consistent nonlocal feedback theory for the phoretic propulsion mechanisms of electrocatalytic micromotors or nanomotors. These swimmers, such as bimetallic platinum and gold rods catalyzing decomposition of hydrogen peroxide in aqueous solution, have received considerable theoretical attention. In contrast, the heterogeneous electrochemical processes with nonlocal feedback that are the actual "engines" of such motors are relatively neglected. We present a flexible approach to these processes using bias potential as a control parameter field and a locally-open-circuit reference state, carried through in detail for a spherical motor. While the phenomenological flavor makes meaningful contact with experiment easier, required inputs can also conceivably come from, e.g., Frumkin-Butler-Volmer kinetics. Previously obtained results are recovered in the weak-heterogeneity limit and improved small-basis approximations tailored to structural heterogeneity are presented. Under the assumption of weak inhomogeneity, a scaling form is deduced for motor speed as a function of fuel concentration and swimmer size. We argue that this form should be robust and demonstrate a good fit to experimental data.

Selectively manipulable acoustic-powered microswimmers.

Selective actuation of a single microswimmer from within a diverse group would be a first step toward collaborative guided action by a group of swimmers. Here we describe a new class of microswimmer that accomplishes this goal. Our swimmer design overcomes the commonly-held design paradigm that microswimmers must use non-reciprocal motion to achieve propulsion; instead, the swimmer is propelled by oscillatory motion of an air bubble trapped within the swimmer's polymer body. This oscillatory motion is driven by the application of a low-power acoustic field, which is biocompatible with biological samples and with the ambient liquid. This acoustically-powered microswimmer accomplishes controllable and rapid translational and rotational motion, even in highly viscous liquids (with viscosity 6,000 times higher than that of water). And by using a group of swimmers each with a unique bubble size (and resulting unique resonance frequencies), selective actuation of a single swimmer from among the group can be readily achieved.