Particle Size-Dependent Electrophoresis in Polymer Solutions.

It has long been known that the electrophoretic velocity of a charged particle is independent of its size under the thin-Debye-layer limit. This so-called Smoluchowski velocity is, however, valid only for Newtonian fluids. A couple of recent theoretical studies predict the rheology-induced particle size dependence of electrophoresis in non-Newtonian fluids. This work presents the first experimental demonstration of such dependence in viscoelastic poly(ethylene oxide) (PEO) solutions. Three different-sized particles are observed to travel at the same electrophoretic velocity in a Newtonian buffer through a rectangular microchannel. In contrast, their measured electrophoretic velocities in the PEO solution exhibit an increasing trend for larger particles, which is consistent with theoretical prediction. This particle size dependence is found to grow with an increasing concentration or length of the PEO polymer. Both trends are attributed to enhanced fluid elasticity, as characterized by the increasing elasticity number.

Effects of Tween 20 addition on electrokinetic transport in a polydimethylsiloxane microchannel.

Tween 20 is frequently added to particle suspensions for reducing the particle-wall adhesion and particle-particle aggregation in microfluidic devices. However, the influences of Tween 20 on the fluid and particle behaviors have been largely ignored. We present in this work the first experimental study of the effects of Tween 20 addition on the electrokinetic transport of fluids and particles in a polydimethylsiloxane microchannel. We find that adding 0.1% v/v Tween 20 to a buffer solution can significantly reduce the electroosmotic mobility as well as the electrokinetic and electrophoretic mobilities of polystyrene particles and yeast cells. Further increasing the Tween 20 concentration within the range typically used in microfluidic applications continues reducing these mobility values, but at a smaller rate. Our finding suggests that Tween 20 should be used with care in electrokinetic microdevices when the flow rate or particle/cell throughput is an important parameter.

Elasto-inertial instabilities in the merging flow of viscoelastic fluids.

Many engineering and natural phenomena involve the merging of two fluid streams through a T-junction. Previous studies of such merging flows have been focused primarily upon Newtonian fluids. We observed in our recent experiment with five different polymer solutions a direct change from an undisturbed to either a steady vortical or unsteady three-dimensional flow at the T-junction with increasing inertia. The transition state(s) in between these two types of merging flow patterns is, however, yet to be known. We present here a systematic experimental study of the merging flow of polyethylene oxide (PEO) solutions with varying polymer concentrations and molecular weights. Two new paths of flow development are identified with the increase of Reynolds number: one is the transition in very weakly viscoelastic fluids first to steady vortical flow and then to a juxtaposition state with an unsteady elastic eddy zone in the middle and a steady inertial vortex on each side, and the other is the transition in weakly viscoelastic fluids first to a steady vortical and/or a juxtaposition state and then to a fully unsteady flow. Interestingly, the threshold Reynolds number for the onset of elastic instabilities in the merging flow is not a monotonic function of the elasticity number, but instead follows a power-law dependence on the polymer concentration relative to its overlap value. Such a dependence turns out qualitatively consistent with the prediction of the McKinley-Pakdel criterion.

Fluid Elasticity-Enhanced Insulator-Based Dielectrophoresis for Sheath-Free Particle Focusing in Very Dilute Polymer Solutions.

Focusing particles into a narrow stream is usually a necessary step in microfluidic flow cytometry and particle sorting. We demonstrate that the addition of a small amount of poly(ethylene oxide) (PEO) polymer into a buffer solution can reduce by almost 1 order of magnitude the threshold DC electric field for single-line dielectrophoretic focusing of particles in a constricted microchannel. The particle focusing effectiveness of this fluid elasticity-enhanced insulator-based dielectrophoresis (E-iDEP) in very dilute PEO solutions gets enhanced with the increase of the PEO molecular weight and particle size. These two trends are consistent with a theoretical analysis that accounts for the fluid elasticity effects on the electrokinetic and dielectrophoretic particle motions. Surprisingly, the particle-focusing effectiveness of E-iDEP is observed to first increase and then decrease with an increase in the PEO concentration.

Nonlinear electrophoresis of nonspherical particles in a rectangular microchannel.

Nonlinear electrophoresis offers advantageous prospects in microfluidic manipulation of particles over linear electrophoresis. Existing theories established for this phenomenon are entirely based on spherical particle models, some of which have been experimentally verified. However, there is no knowledge on if and how the particle shape may affect the nonlinear electrophoretic behavior. This work presents an experimental study of the nonlinear electrophoretic velocities of rigid peanut- and pear-shaped particles in a rectangular microchannel, which are compared with rigid spherical particles of similar diameter and surface charge in terms of the particle slenderness. We observe a decrease in the nonlinear electrophoretic mobility, whereas an increase in the nonlinear index of electric field when the particle slenderness increases from the peanut- to pear-shaped and spherical particles. The values of the nonlinear index for the nonspherical particles are, however, still within the theoretically predicted range for spherical particles. We also observe an enhanced nonlinear electrophoretic behavior in a lower concentration buffer solution regardless of the particle shape.

Recent advances in multimode microfluidic separation of particles and cells.

Microfluidic separation of particles and cells is crucial to lab-on-a-chip applications in the fields of science, engineering, and industry. The continuous-flow separation methods can be classified as active or passive depending on whether the force involved in the process is externally imposed or internally induced. The majority of current separations have been realized using only one of the active or passive methods. Such a single-mode process is usually limited to one-parameter separation, which often becomes less effective or even ineffective when dealing with real samples because of their inherent heterogeneity. Integrating two or more separation methods of either type has been demonstrated to offer several advantages like improved specificity, resolution, and throughput. This article reviews the recent advances of such multimode particle and cell separations in microfluidic devices, including the serial-mode prefocused separation, serial-mode multistage separation, and parallel-mode force-tuned separation.

Nonlinear electrophoresis of dielectric particles in Newtonian fluids.

In classical electrokinetics, the electrophoretic velocity of a dielectric particle is a linear function of the applied electric field. Theoretical studies have predicted the onset of nonlinear electrophoresis at high electric fields because of the nonuniform surface conduction over the curved particle. However, experimental studies have been left behind and are insufficient for a fundamental understanding of the parametric effects on nonlinear electrophoresis. We present in this work a systematic experimental study of the effects of buffer concentration, particle size, and particle zeta potential on the electrophoretic velocity of polystyrene particles in a straight rectangular microchannel for electric fields of up to 3 kV/cm. The measured nonlinear electrophoretic particle velocity is found to exhibit a 2(±0.5)-order dependence on the applied electric field, which appears to be within the theoretically predicted 3- and 3/2-order dependences for low and high electric fields, respectively. Moreover, the obtained nonlinear electrophoretic particle mobility increases with decreasing buffer concentration (for the same particle) and particle size (for particles with similar zeta potentials) or increasing particle zeta potential (for particles with similar sizes). These observations are all consistent with the theoretical predictions for high electric fields.

An experimental study of the merging flow of polymer solutions in a T-shaped microchannel.

The merging flow through a T-junction is relevant to sample mixing and particle manipulation in microfluidic devices. It has been extensively studied for Newtonian fluids, particularly in the high inertial regime where flow bifurcation takes place for enhanced mixing. However, the effects of fluid rheological properties on the merging flow have remained largely unexplored. We investigate here the flow of five types of polymer solutions along with water in a planar T-shaped microchannel over a wide range of flow rates for a systematic understanding of the effects of fluid shear thinning and elasticity. It is found that the merging flow near the stagnation point of the T-junction can either be vortex dominated or have unsteady streamlines, depending on the strength of elasticity and shear thinning present in the fluid. Moreover, the shear thinning effect is found to induce a symmetric unsteady flow in comparison to the asymmetric unsteady flow in the viscoelastic fluids, the latter of which exhibits greater interfacial fluctuations.

Review of nonlinear electrokinetic flows in insulator-based dielectrophoresis: From induced charge to Joule heating effects.

Insulator-based dielectrophoresis (iDEP) has been increasingly used for particle manipulation in various microfluidic applications. It exploits insulating structures to constrict and/or curve electric field lines to generate field gradients for particle dielectrophoresis. However, the presence of these insulators, especially those with sharp edges, causes two nonlinear electrokinetic flows, which, if sufficiently strong, may disturb the otherwise linear electrokinetic motion of particles and affect the iDEP performance. One is induced charge electroosmotic (ICEO) flow because of the polarization of the insulators, and the other is electrothermal flow because of the amplified Joule heating in the fluid around the insulators. Both flows vary nonlinearly with the applied electric field (either DC or AC) and exhibit in the form of fluid vortices, which have been utilized to promote some applications while being suppressed in others. The effectiveness of iDEP benefits from a comprehensive understanding of the nonlinear electrokinetic flows, which is complicated by the involvement of the entire iDEP device into electric polarization and thermal diffusion. This article is aimed to review the works on both the fundamentals and applications of ICEO and electrothermal flows in iDEP microdevices. A personal perspective of some future research directions in the field is also given.

Fluid rheological effects on streaming dielectrophoresis in a post-array microchannel.

Recent studies have demonstrated the strong influences of fluid rheological properties on insulator-based dielectrophoresis (iDEP) in single-constriction microchannels. However, it is yet to be understood how iDEP in non-Newtonian fluids depends on the geometry of insulating structures. We report in this work an experimental study of fluid rheological effects on streaming DEP in a post-array microchannel that presents multiple contractions and expansions. The iDEP focusing and trapping of particles in a viscoelastic polyethylene oxide solution are comparable to those in a Newtonian buffer, which is consistent with the observations in a single-constriction microchannel. Similarly, the insignificant iDEP effects in a shear-thinning xanthan gum solution also agree with those in the single-constriction channel except that gel-like structures are observed to only form in the post-array microchannel under large DC electric fields. In contrast, the iDEP effects in both viscoelastic and shear-thinning polyacrylamide solution are significantly weaker than in the single-constriction channel. Moreover, instabilities occur in the electroosmotic flow and appear to be only dependent on the DC electric field. These phenomena may be associated with the dynamics of polymers as they are electrokinetically advected around and through the posts.

Effects of vertical confinement on the flow of polymer solutions in planar constriction microchannels.

The flow of polymer solutions under extensional conditions is frequently encountered in numerous engineering fields. Planar contraction and/or expansion microchannels have been a subject of interest for many studies in that regard, which, however, have mostly focused on shallow channel structures. We investigate here the effect of changing the depth of contraction-expansion microchannels on the flow responses of three types of polymer solutions and water. The flow of viscoelastic polyethylene oxide (PEO) solution is found to become more stable with suppressed vortex formation and growth in the contraction part while being less stable in the expansion part with the increase of the channel depth. These opposing trends in the contraction and expansion flows are noted to have similarities with our recent findings of constriction length-dependent instabilities in the same PEO solution (M. K. Raihan, S. Wu, Y. Song and X. Xuan, Soft Matter, 2021, 17, 9198-9209), where the contraction flow gets stabilized while the expansion flow becomes destabilized with the increase of the constriction length. In contrast, the entire flow becomes less stable in deeper channels for the shear-thinning xanthan gum (XG) solution as well as the shear thinning and viscoelastic polyacrylamide (PAA) solution. This observation aligns with that of water flow, which is attributed to the reduced top/bottom wall stabilizing effects.

AC Insulator-Based Dielectrophoretic Focusing of Particles and Cells in an "Infinite" Microchannel.

It is often necessary to prefocus particles and cells into a tight stream for subsequent separation and/or analysis in microfluidic devices. A DC electric field has been widely used for particle and cell focusing in insulator-based dielectrophoretic (iDEP) microdevices, where a large field magnitude, a high constriction ratio, and/or a long microchannel are usually required to enhance the iDEP effect. We demonstrate, in this work, an AC iDEP focusing technique, which utilizes a low-frequency AC electric field to generate both an oscillatory electrokinetic flow of the particle/cell suspension and a field direction-independent dielectrophoretic force for particle/cell focusing in a virtually "infinite" microchannel. We also develop a theoretical analysis to evaluate this focusing in terms of the AC voltage frequency, amplitude, and particle size, which are each validated through both experimental demonstration and numerical simulation. The effectiveness of AC iDEP focusing increases with the second order of electric field magnitude, superior to DC iDEP focusing with only a first-order dependence. This feature and the "infinite" channel length together remove the necessity of large electric field and/or small constriction in DC iDEP focusing of small particles.

Joule heating effects on electrokinetic flows with conductivity gradients.

Instability occurs in the electrokinetic flow of fluids with conductivity and/or permittivity gradients if the applied electric field is beyond a critical value. Understanding such an electrokinetic instability is significant for both improved transport (via the suppressed instability) and enhanced mixing (via the promoted instability) of liquid samples in microfluidic applications. This work presents the first study of Joule heating effects on electrokinetic microchannel flows with conductivity gradients using a combined experimental and numerical method. The experimentally observed flow patterns and measured critical electric fields under Joule heating effects to different extents are reasonably predicted by a depth-averaged numerical model. It is found that Joule heating increases the critical electric field for the onset of electrokinetic instability because the induced fluid temperature rise and in turn the fluid property change (primarily the decreased permittivity) lead to a smaller electric Rayleigh number.

Joule heating-enabled electrothermal enrichment of nanoparticles in insulator-based dielectrophoretic microdevices.

Insulator-based dielectrophoresis (iDEP) exploits the electric field gradients formed around insulating structures to manipulate particles for diverse microfluidic applications. Compared to the traditional electrode-based dielectrophoresis, iDEP microdevices have the advantages of easy fabrication, free of water electrolysis, and robust structure, etc. However, the presence of in-channel insulators may cause thermal effects because of the locally amplified Joule heating of the fluid. The resulting electrothermal flow circulations are exploited in this work to trap and concentrate nanoscale particles (of 100 nm diameter and less) in a ratchet-based iDEP microdevice. Such Joule heating-enabled electrothermal enrichment of nanoparticles are found to grow with the increase of alternating current or direct current electric field. It also becomes more effective for larger particles and in a microchannel with symmetric ratchets. Moreover, a depth-averaged numerical model is developed to understand and simulate the various parametric effects, which is found to predict the experimental observations with a good agreement.

Insulator-based dielectrophoretic focusing and trapping of particles in non-Newtonian fluids.

Insulator-based dielectrophoretic (iDEP) microdevices have been limited to work with Newtonian fluids. We report an experimental study of the fluid rheological effects on iDEP focusing and trapping of polystyrene particles in polyethylene oxide, xanthan gum, and polyacrylamide solutions through a constricted microchannel. Particle focusing and trapping in the mildly viscoelastic polyethylene oxide solution are slightly weaker than in the Newtonian buffer. They are, however, significantly improved in the strongly viscoelastic and shear thinning polyacrylamide solution. These observed particle focusing behaviors exhibit a similar trend with respect to electric field, consistent with a revised theoretical analysis for iDEP focusing in non-Newtonian fluids. No apparent focusing of particles is achieved in the xanthan gum solution, though the iDEP trapping can take place under a much larger electric field than the other fluids. This is attributed to the strong shear thinning-induced influences on both the electroosmotic flow and electrokinetic/dielectrophoretic motions.

Constriction length dependent instabilities in the microfluidic entry flow of polymer solutions.

Transport phenomena of fluids and particles through contraction and/or expansion geometries have relevance in many applications. Polymer solutions are often the transporter in these processes, giving rise to flow complexities. The separation distance between a contraction and a following expansion in microfluidic entry flow can affect the interplay between the shear and extension force dominated flow regimes, but the process is still little understood. We investigate the rheological responses of such constriction length dependent instabilities with three different polymer solutions and water in planar contraction-expansion microchannels differing only in the constriction length. The viscoelastic polyethylene oxide (PEO) solution is found to exhibit strong constriction length-dependent instabilities in both the contraction and expansion flows. Such a dependence is, however, completely absent from the flow of shear-thinning xanthan gum (XG) solution and Newtonian water. Interestingly, it is only present in the expansion flow of the both shear thinning and viscoelastic polyacrylamide (PAA) solution.

Elastic instabilities in the electroosmotic flow of non-Newtonian fluids through T-shaped microchannels.

Electroosmotic flow (EOF) has been widely used to transport fluids and samples in micro- and nanofluidic channels for lab-on-a-chip applications. This essentially surface-driven plug-like flow is, however, sensitive to both the fluid and wall properties, of which any inhomogeneity may draw disturbances to the flow and even instabilities. Existing studies on EOF instabilities have been focused primarily upon Newtonian fluids though many of the chemical and biological solutions are actually non-Newtonian. We carry out a systematic experimental investigation of the fluid rheological effects on the elastic instability in the EOF of phosphate buffer-based polymer solutions through T-shaped microchannels. We find that electro-elastic instabilities can be induced in shear thinning polyacrylamide (PAA) and xanthan gum (XG) solutions if the applied direct current voltage is above a threshold value. However, no instabilities are observed in Newtonian or weakly shear thinning viscoelastic fluids including polyethylene oxide (PEO), polyvinylpyrrolidone (PVP), and hyaluronic acid (HA) solutions. We also perform a quantitative analysis of the wave parameters for the observed elasto-elastic instabilities.

Recent advances in direct current electrokinetic manipulation of particles for microfluidic applications.

Microfluidic devices have been extensively used to achieve precise transport and placement of a variety of particles for numerous applications. A range of force fields have thus far been demonstrated to control the motion of particles in microchannels. Among them, electric field-driven particle manipulation may be the most popular and versatile technique because of its general applicability and adaptability as well as the ease of operation and integration into lab-on-a-chip systems. This article is aimed to review the recent advances in direct current (DC) (and as well DC-biased alternating current) electrokinetic manipulation of particles for microfluidic applications. The electric voltages are applied through electrodes that are positioned into the distant channel-end reservoirs for a concurrent transport of the suspending fluid and manipulation of the suspended particles. The focus of this review is upon the cross-stream nonlinear electrokinetic motions of particles in the linear electroosmotic flow of fluids, which enable the diverse control of particle transport in microchannels via the wall-induced electrical lift and/or the insulating structure-induced dielectrophoretic force.

Revisit of wall-induced lateral migration in particle electrophoresis through a straight rectangular microchannel: Effects of particle zeta potential.

Previous studies have reported a lateral migration in particle electrophoresis through a straight rectangular microchannel. This phenomenon arises from the inherent wall-induced electrical lift that can be exploited to focus and separate particles for microfluidic applications. Such a dielectrophoretic-like force has been recently found to vary with the buffer concentration. We demonstrate in this work that the particle zeta potential also has a significant effect on the wall-induced electrical lift. We perform an experimental study of the lateral migration of equal-sized polystyrene particles with varying surface charges under identical electrokinetic flow conditions. Surprisingly, an enhanced focusing is observed for particles with a faster electrokinetic motion, which indicates a substantially larger electrical lift for particles with a smaller zeta potential. We speculate this phenomenon may be correlated with the particle surface conduction that is a strong function of particle and fluid properties.

Electroosmotic flow of non-Newtonian fluids in a constriction microchannel.

Insulator-based dielectrophoresis has to date been almost entirely restricted to Newtonian fluids despite the fact that many of the chemical and biological fluids exhibit non-Newtonian characteristics. We present herein an experimental study of the fluid rheological effects on the electroosmotic flow of four types of polymer solutions, i.e., 2000 ppm xanthan gum (XG), 5% polyvinylpyrrolidone (PVP), 3000 ppm polyethylene oxide (PEO), and 200 ppm polyacrylamide (PAA) solutions, through a constriction microchannel under DC electric fields of up to 400 V/cm. We find using particle streakline imaging that the fluid elasticity does not change significantly the electroosmotic flow pattern of weakly shear-thinning PVP and PEO solutions from that of a Newtonian solution. In contrast, the fluid shear-thinning causes multiple pairs of flow circulations in the weakly elastic XG solution, leading to a central jet with a significantly enhanced speed from before to after the channel constriction. These flow vortices are, however, suppressed in the strongly viscoelastic and shear-thinning PAA solution.