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Here, we report on a new class active particles capable of dynamically programmable motion powered by electricity. We have implemented physical principles that separate the propulsion and steering mechanisms of active motion using optically activated, patterned, photoresponsive semiconductor coatings on intricate microstructures. Our engineered microswimmer robots employ an induced-charge electro-phoresis (ICEP) mechanism to achieve linear motion and optically modulated electrokinetic propulsion (OMEP) for steering. Optical modulation is achieved by manipulating the polarizability of patterned ZnO semiconductor coating through exposure to light with wavelengths above its bandgap, exploiting the semiconductor's photoconductive properties. Unlike previous methods that rely on changing the direction of optical illumination or spatially controlling narrow optical beams, our approach achieves optical steering under uniform ambient illumination conditions, thereby greatly reducing the complexity of the optical system. The decoupling of propulsion and steering allows for the programming of micromotor trajectories in both open and closed-loop control modes. We anticipate that our findings will pave the way for efficient optically gated control of the trajectory of photoresponsive active particles. Furthermore, they will enable the selective manipulation of specific subgroups of engineered active microparticles with various semiconducting coatings having different band gaps.

Self-propelling active particles are an exciting and interdisciplinary emerging area of research with projected biomedical and environmental applications. Due to their autonomous motion, control over these active particles that are free to travel along individual trajectories, is challenging. This work used optically patterned electrodes on a photoconductive substrate using a digital micromirror device (DMD) to dynamically control the region of movement of self-propelling particles (i.e. metallo-dielectric Janus particles (JPs)). This extends previous studies where only a passive micromotor was optoelectronically manipulated with a translocating optical pattern that illuminated the particle. In contrast, the current system used the optically patterned electrode merely to define the region within which the JPs moved autonomously. Interestingly, the JPs avoided crossing the optical region edge, which enables constraint of the area of motion and to dynamically shape the JP trajectory. Using the DMD system to simultaneously manipulate several JPs enabled to self-assemble the JPs into stable active structures (JPs ring) with precise control over the number of participating JPs and passive particles. Since the optoelectronic system is amenable to closed-loop operation using real-time image analysis, it enables exploitation of these active particles as active microrobots that can be operated in a programmable and parallelized manner

Electrically powered micro- and nanomotors are promising tools for in-vitro single-cell analysis. In particular, single cells can be trapped, transported and electroporated by a Janus particle (JP) using an externally applied electric field. However, while dielectrophoretic (DEP)-based cargo manipulation can be achieved at high-solution conductivity, electrical propulsion of these micromotors becomes ineffective at solution conductivities exceeding 0.3mS/cm. Here, we successfully extended JP cargo manipulation and transport capabilities to conductive near-physiological (<6mS/cm) solutions by combining magnetic field-based micromotor propulsion and navigation with DEP-based manipulation of various synthetic and biological cargos. Combination of a rotating magnetic field and electric field resulted in enhanced micromotor mobility and steering control through tuning of the electric field frequency. conditions are necessary. In addition, we demonstrated the micromotors ability of identifying apoptotic cell among viable and necrotic cells based their dielectrophoretic difference, thus, enabling to analyze the apoptotic status in the single cell samples for drug discovery, cell therapeutics and immunotherapy. We also demonstrated the ability to trap and transport live cells towards regions containing doxorubicin-loaded liposomes. This hybrid micromotor approach for label-free trapping, transporting and sensing of selected cells within conductive solutions, opens new opportunities in drug delivery and single cell analysis, where close-to-physiological media

The electro-rotation (EROT) and electro-orientation (EOR) behavior of metallodielectric (MD) 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 a 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 angular velocity on the forcing frequency of a rotating and non-rotating spatially uniform electric field, respectively, are explicitly determined and compared against experiments (different JP size and solution conductivity). A favorably good qualitative agreement between theory and experimental measurements was found.

This article presents the implementation of on-chip iontronic circuits via small-scale integration of multiple ionic logic gates made of bi-polar polyelectrolyte diodes. These ionic circuits are analogous to solid-state electronic circuits, with ions as the charge carriers instead of electrons/holes. We experimentally characterize the responses of a single fluidic diode made of a junction of oppositely charged polyelectrolytes (i.e., anion and cation exchange membranes), with a similar underlying mechanism as a solid-state p- and n-type junction. This served to carry out pre-designed logical computations in various architectures by integrating multiple diode-based logic gates, where the electrical signal between the integrated gates was transmitted entirely through ions. The findings shed light on the limitations affecting the number of logic gates that can be integrated, the degradation of the electrical signal, their transient response, and the design rules that can improve the performance of iontronic circuits.

Microfluidic channels with embedded ion permselective medium under the application of electric current are commonly used for electrokinetic processes as on-chip ion concentration polarization (ICP) and bioparticle preconcentration to enhance biosensing. Herein, we demonstrate the ability to dynamically control the electrically driven ion transport by integrating individually addressable microvalves. The microvalves are located along a main microchannel that is uniformly coated with a thin layer of an ion-exchange membrane (IEM). The interplay of ionic transport between the solution within the microchannel and the thin IEM, under an applied electric current, can be locally tuned by the deformation of the microvalve. This tunability provides a robust and simple means of implementing new functionalities into lab-on-a-chip devices, e.g., dynamic control over multiple ICP layers and their associated preconcentrated molecule plugs, multiplex sensing, suppression of biofouling as well as plug dispersion, while maintaining the well-known application of microvalves as steric filtration.

Herein we demonstrate the ability to optically tune the mobility of electrically powered Janus particles (JP) that are half coated with various Zinc Oxide (ZnO) semiconducting layers, i.e. polycrystalline, amorphous and amorphous with a SiO2 passivation layer. The ZnO semiconductor photo-response enables increase in its electrical conductivity with light having wavelengths of sufficient photon energy with respect to the semiconductor bandgap. This effect, termed optically modulated electrokinetic propulsion (OMEP), can be harnessed to increase the contrast in polarizability between the dielectric and semiconducting hemispheres, which in turn, results in an increased electrokinetic mobility. The addition of optical activation to the electrical field enables an additional degree of control of JP mobility. We also demonstrate optical control of collective behavior and particle-particle interactions for dense semi-conducting Janus particle populations.

Ionic concentration-polarization (CP)-based biomolecule preconcentration is an established method for enhancing the detection sensitivity of target biomolecules. However, the formed preconcentrated biomolecule plug rapidly sweeps over the surface-immobilized antibodies, resulting in a short-term overlap between the capture agent and the analyte, and subsequently suboptimal binding. To overcome this, we designed a setup allowing for periodic formation of a preconcentrated biomolecule plug by activating the CP for predetermined on/off intervals. This work demonstrated the feasibility of the cyclic CP actuation and optimized the sweeping conditions required to obtain maximum retention time of a preconcentrated plug over a desired sensing region and enhanced detection sensitivity. The ability of this method to efficiently preconcentrate different analytes and to successfully increase immunoassay sensitivity, underscore its potential in immunoassays serving the clinical and food testing industries.

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., Comment: 10 pages, 4 figures

Self-propelling micromotors are emerging as a promising microscale and nanoscale tool for single-cell analysis. We have recently shown that the field gradients necessary to manipulate matter via dielectrophoresis can be induced at the surface of a polarizable active (self-propelling) metallo-dielectric Janus particle (JP) under an externally applied electric field, acting essentially as a mobile floating microelectrode. Here, we successfully demonstrated for the first time, that the application of an external electric field can singularly trap and transport bacteria and can selectively electroporate the trapped bacteria. Selective electroporation, enabled by the local intensification of the electric field induced by the JP, was obtained under both continuous alternating current and pulsed signal conditions. This approach is generic and is applicable to bacteria and JP, as well as a wide range of cell types and micromotor designs. Hence, it constitutes an important and novel experimental tool for single-cell analysis and targeted delivery.

The use of active colloids for cargo transport offers unique potential for applications ranging from targeted drug delivery to lab-on-a-chip systems. Previously, Janus particles (JPs), acting as mobile microelectrodes have been shown to transport cargo which is trapped by a dielectrophoretic mechanism [Boymelgreen et al. (2018)]. Herein, we aim to characterize the cargo loading properties of mobile Janus carriers, across a broad range of frequencies and voltages. In expanding the frequency range of the carrier, we are able to compare the influence of different modes of carrier transport on the loading capacity as well as highlight the differences between cargo trapped by positive and negative dielectrophoresis. Specifically it is shown that cargo trapping results in a reduction in carrier velocities with this effect more pronounced at low frequencies where cargo is trapped close to the substrate. Interestingly, we observe the existence of a maximum cargo loading capacity which decreases at large voltages suggesting a strong interplay between trapping and hydrodynamic shear. Finally, we demonstrate that control of the frequency can enable different assemblies of binary colloidal solutions on the JP. The resultant findings enable the optimization of electrokinetic cargo transport and its selective application to a broad range of targets.

Concentration polarization (CP) based biomolecule preconcentration is highly effective in enhancing the detection sensitivity, yet fails to precisely and dynamically control the location of the preconcentrated biomolecule plug to ensure overlap with the sensing region (e.g. immobilized molecular probes). Here, we used electrothermal (ET) stirring as a means of controlling the location of a preconcentrated biomolecule plug. The applied microfluidic device consisted of a Nafion membrane to induce the CP, and an array of individually addressable microscale heaters for active local ET stirring. The experimental results demonstrated that such a novel platform enabled active control of the location of the preconcentrated plug of target biomolecules, ensuring its overlap with the functionalized microparticles, ultimately yielding enhanced detection sensitivity and binding kinetics. This was demonstrated using avidin-biotin particles as a simple bead-based bioassay model.

The ability to induce regions of high and low ionic concentration adjacent to a permeselective membrane or nanochannel subject to an externally applied electric field (a phenomenon termed concentration-polarization) has been used for a broad spectrum of applications ranging from on-chip desalination, bacteria filtration to biomolecule preconcentration. But these applications have been limited by the ability to control the length of the diffusion layer that is commonly indirectly prescribed by the fixed geometric and surface properties of the nanofluidic system. Here, we demonstrate that the depletion layer can be dynamically varied by inducing controlled electrothermal flow driven by the interaction of temperature gradients with the applied electric field. To this end, a series of microscale heaters, which can be individually activated on demand are embedded at the bottom of the microchannel and the relationship between their activation and ionic concentration is characterized. Such spatio-temporal control of the diffusion layer can be used to enhance on-chip electro-dialysis by producing shorter depletion layers, to dynamically reduce the microchannel resistance relative to that of the nanochannel for nanochannel based (bio)sensing, to generate current rectification reminiscent of a diode like behavior and control the location of the preconcentrated plug of analytes or the interface of brine and desalted streams.

With an eye towards next-generation, smart, micro/nanofluidic devices, capable of responding to external stimuli or changes in environment, we demonstrate a means to achieve dynamic control of the spatio-temporal properties of the electric field in a standardized microfluidic chamber. Typical top-down patterning, currently used to design the field distribution, is replaced by freely-suspended colloids which locally disturb the electric field from the bottom-up. Even under uniform forcing, polarization of the colloid induces the formation of strong, three-dimensional gradients at its surface - essentially repurposing it into a portable floating electrode whose precise location can be manipulated to reconfigure the electric field in real time. Focusing on active Janus colloids as a sample platform, we measure the strength of the induced gradients and highlight the advantages of a colloid-based system by revealing a prototype for an all-in-one cargo carrier, capable of on-demand, selective, label-free assembly and transport of micro/nano sized targets.

The current study extends previous analytical and numerical solutions of chronopotentiometric response of one-dimensional systems consisting of three layers to the more realistic two-dimensional heterogeneous ion-permselective medium. An analytical solution for the transient concentration-polarization problem, under the local electro-neutrality approximation and ideal permselectivity, was obtained using the Laplace transform and separation of variables. Then the two-dimensional electric potential was obtained numerically and was compared to the full Poisson-Nernst-Planck solution. It was then shown that the resultant voltage drop across the system varies between the initial Ohmic response and that of the steady-state accounting for concentration-polarization. Also, field-focusing effect in a two-dimensional system is shown to result in a faster depletion of ions at the permselective interface., Comment: Submitted to Phys. Rev. E. Includes 6 figures

We demonstrate the role of selectivity variation in the structure of the non-equilibrium extended space-charge using 1D analytic and 2D numerical Poisson-Nernst-Planck models for the electro- diffusive transport of a symmetric electrolyte. This provides a deeper understanding of the underly- ing mechanism behind a previously-observed maximum in the resistance-voltage curve for a shallow micro-nanochannel interface device [Schiffbauer, Liel, Leibowitz, Park, and Yossifon, submitted to Phys. Rev. E.]. The current study helps to establish a connection between parameters such as the geometry and nanochannel surface-charge and the control of selectivity and resistance in the over-limiting current regime.

Induced-charge electro-osmosis (ICEO) is shown to control the length scale of the diffusion layer (DL), which in turn, affects the diffusion limited ion transport through the microchannel-Nafion membrane system. The ICEO vortices form at an interdigitated floating electrode array embedded within a microchannel interfacing a Nafion membrane and stir the fluid, arresting the diffusive growth of the depletion layer. By varying the spacing between the array and the membrane we are able to control the length of the DL. Activating the electrodes results in further enhancement of the fluid stirring due to the emergence of alternating-current electro-osmotic (ACEO) flow on top of the ICEO. Such a new method of controlling the DL with an electrode array is of great importance in many CP related realizations.

The microchannel corner is a common inherent component of most planar microfluidic systems and thus its influence on the channel flow is of significant interest. Application of an alternating current electric field enables quantification of the non-linear induced-charge electro-osmosis (ICEO) ejection flow effect by isolating it from linear electro-osmotic background flow which is present under dc forcing. The hydrodynamic flow in the vicinity of a sharp channel corner is analyzed using experimental micro-particle-image-velocimetry (PIV) and numerical simulations for different buffer concentrations, frequencies and applied voltages. Divergence from the purely ICEO flow with increasing buffer conductivity is shown to be a result of increasing electro-thermal effects due to Joule heating.

To bridge the gap between single/isolated pore systems to multi-pore systems, such as membranes/electrodes, we studied an array of nanochannels with varying interchannel spacing that controlled the degree of channel communication. Instead of treating them as individual channels connected in parallel or an assembly like a homogeneous membrane, this study resolves the pore-pore interaction. We found that increased channel isolation leads to current intensification whereas at high voltages electro-convective effects control the degree of communication via suppression of the diffusion layer growth, Comment: 4 figures,submitted to Phys. Rev. E

We present results demonstrating the space charge-mediated transition between classical, diffusion-limited current and surface-conduction dominant over-limiting current in a shallow micro-nanochannel device. The extended space charge layer develops at the depleted micro-nanochannel entrance at high current and is correlated with a distinctive maximum in the dc resistance. Experimental results for a shallow surface-conduction dominated system are compared with theoretical models, allowing estimates of the effective surface charge at high voltage to be obtained. In comparison to an equilibrium estimate of the surface charge obtained from electrochemical impedance spectroscopy, it is further observed that the effective surface charge appears to change under applied voltage.

This study extends previous analytical solutions of concentration-polarization occurring solely in the depleted region, to the more realistic geometry consisting of a three dimensional (3D) heterogeneous ion-permselective medium connecting two opposite microchambers (i.e. 3 layers system). Under the local electro-neutrality approximation, the separation of variable methods is used to derive an analytical solution of the electro-diffusive problem for the two opposing asymmetric microchambers. Assuming an ideal permselective medium allows for the analytic calculation of the 3D concentration and electric potential distributions as well as a current-voltage relation. It is shown that any asymmetry in the microchamber geometries will result in current rectification. Moreover, it is demonstrated that for non-negligible microchamber resistances the conductance does not exhibit the expected saturation at low concentrations but instead shows a continuous decrease. The results are intended to facilitate a more direct comparison between theory and experiments as now the voltage drop is across a realistic 3D and 3-layer system., Comment: 7 figures

We study here the curious particle dynamics resulting from electro-osmotic flow around a microchannel junction corner whose dielectric walls are weakly polarizable. The hydrodynamic velocity field is obtained via superposition of a linear irrotational term associated with the equilibrium zeta potentials of both the microchannel and particle surfaces and the non-linear induced-charge electro-osmotic flow which originates from the interaction of the externally applied electric field on the charge cloud it induces at the solid-liquid interface. The particle dynamics are analyzed by considering dielectrophoretic forces via the addition of a mobility term to the flow field in the limit of Stokes drag law. The former, non-divergence free term is responsible for migration of particles towards the sharp microchannel junction corner, where they can potentially accumulate. Experimental observations of particle trapping for various applied electric fields and microparticle size are rationalized in terms of the growing relative importance of the dielectrophoretic force and induced-charge contributions to the global velocity field with increasing intensity of the externally applied electric field.

We provide an experimental proof-of-concept for a robust, continuously rotating microstructure - consisting of two metallodielectric (gold-polystyrene)Janus particles rigidly attached to each other - which is driven in uniform ac fields by asymmetric induced-charge electroosmosis. The pairs (doublets) are stabilized on the substrate surface which is parallel to the plane of view and normal to the direction of the applied electric field. We find that the radius of orbit and angular velocity of the pair are predominantly dependent on the relative orientations of the interfaces between the metallic and dielectric hemispheres and that the electrohydrodynamic particle-particle interactions are small. Additionally, we verify that both the angular and linear velocities of the pair are proportional to the square of the applied field which is consistent with the theory for non-linear electrokinetics. A simple kinematic rigid body model is used to predict the paths and double velocities (angular and linear) based on their relative orientations with good agreement.