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Levitan 2005 Coll Surf a ICE3

Levitan 2005 Coll Surf a ICE3

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Colloids and Surfaces A: Physicochem. Eng. Aspects 267 (2005) 122–132
Experimental observation of induced-charge electro-osmosisaround a metal wire in a microchannel
Jeremy A. Levitan
, Shankar Devasenathipathy
, Vincent Studer
, Yuxing Ben
,Todd Thorsen
, Todd M. Squires
, Martin Z. Bazant
 Institute for Soldier Nanotechnologies, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
 Department of Mechanical Engineering, MIT, Cambridge, MA 02139, USA
 Department of Chemical Engineering, MIT, Cambridge, MA 02139, USA
 Department of Mathematics, MIT, Cambridge, MA 02139, USA
 Laboratoire de Photonique et Nanostructures, CNRS UPR 20 Route de Nozay, Marcoussis, 91460 Paris, France
 Departments of Applied and Computational Mathematics and Physics, California Institute of Technology, Pasadena, CA 91125, USA
Available online 2 August 2005
Induced-charge electro-osmosis (ICEO) is demonstrated around an isolated platinum wire in a polymer microchannel filled with low-concentration KCl, subject to a weak alternating electric field. In contrast to ac electro-osmosis at electrode arrays, which shares the same slipmechanism,ICEOhasamoregeneralfrequencydependence,includingsteadyflowinthedclimit(sincethewireisnotanelectrodedrivingthefield).Theflowprofileinsidethedevice,measuredbyparticleimagevelocimetry,confirmsthepredictedscalingwiththesquareoftheappliedvoltage,aswellasthecharacteristiccut-offfrequency.Aquantitativecomparisonwithnumericalsolutionsofthemodelsequationsisreportedfor various equivalent circuit models from the literature. The standard model of linear capacitors captures the basic trends, but systematicallyover-predicts the velocity. A better fit to experiment can be obtained with a complex impedance, taking into account the frequency dispersionof capacitance, although the microscopic justification of this model is unclear especially in the presence of electro-osmotic flow and appliedvoltages well into the non-linear regime.© 2005 Elsevier B.V. All rights reserved.
Induced-charge electro-osmosis; Non-linear electrokinetics; Equivalent circuit models; Particle image velocimetry; Microfluidics
1. Introduction
Increased access to microfabrication technologies hasspurred growing interest in the possibilities and the benefitsof miniaturization in chemical analysis and biomedicalscreening. Microfluidics holds the promise of ultra-fastbiological assays, analysis of ultra-dilute samples and char-acterization of a previously unrealized compounds[1–3].In principle, these advances could be fully miniaturized,enabling new implantable medical devices and diagnostics,but there is still a need to develop robust techniques forpumping in portable microfluidic devices.
Corresponding author. Tel.: +1 617 253 1713.
 E-mail address:
bazant@mit.edu (M.Z. Bazant).
Conventionalpressure-drivenflowsarecommonlyusedinmicrofluidics[6], as long as the channel dimensions are nottoo small (
m) and they have the advantage of beingrobust and easy to operate, regardless of the fluid composi-tion. Nevertheless, pressure-driven flows have poor scalingwith miniaturization and do not offer simple local control of flow direction and circulation. The pressure gradient neededto maintain a constant fluid velocity increases as the inversesquare of the channel width and rather bulky (non-portable)pressure sources are often required.Electrokineticsoffersanalternativemeanstopressuregra-dients to drive microflows, which is gaining increased atten-tion[4,5].Perhaps,thebestknownexampleofelectrokinetics istheelectrophoresisofchargedcolloidalparticles[7],where anappliedelectricfieldactsondiffusedouble-layerchargeto
0927-7757/$ – see front matter © 2005 Elsevier B.V. All rights reserved.doi:10.1016/j.colsurfa.2005.06.050
 J.A. Levitan et al. / Colloids and Surfaces A: Physicochem. Eng. Aspects 267 (2005) 122–132
produce fluid slip. By the same mechanism, an electric fieldapplied down a glass or polymer microchannel can drive aplug-like flow in capillary electrophoresis.Standard electrokinetic effects are linear in the appliedfield, which presents some disadvantages for microfluidics,especially in miniaturization. Aside from being fairly weak,linear electro-osmotic flows suffer from the requirement of directcurrentandthuselectrochemicalreactionsatelectrodesto maintain a steady flow. Alternating current suppresses re-actions and thus can allow larger driving voltages withoutbubble formation or sample contamination by reaction prod-ucts,butlinearflowstime-averagetozeroinalternatingfields.Another problem for miniaturization is the large power re-quirement of linear electro-osmosis, since the voltage is ap-plied globally down the channel, rather than locally acrossthe channel. As a result, to achieve typical electric fields over100V/cm, one must apply over 100V across a 1cm longmicrofluidic chip. It would be preferable for portable or im-plantablemicrofluidicstomakeuseofthemuchsmallervolt-ages (1–10V) supplied by microbatteries by applying fieldslocally at the scale of the channel width.Non-linear electrokinetic phenomena provide a promis-ing alternative mechanism for flow control in microfluidicdevices. The first non-linear electrokinetic phenomenon de-scribedinthemicrofluidicliteraturewas“acelectro-osmosis”atmicroelectrodearrays,independentlydiscoveredbyRamoset al.[8,9]and Ajdari[10]and studied extensively ever since [11–16].SimilarflowswerealsoobservedbyNadaletal.[17] around a dielectric stripe on an electrode by Thamida andChang[18].Recently, Bazant and Squires[19,20]pointed outthatthephysicalprinciplebehindacelectro-osmosisanelectric field acting on its own induced double-layer chargeat a polarizable surface – is more general, requiring neitherelectrodes nor ac fields and they suggested the more descrip-tive term, “induced-charge electro-osmosis” (ICEO) to de-scribe the basic mechanism. They also noted that essentiallythe same effect had been described earlier in the Russian lit-erature on metallic colloids by Murtsovkin and co-workers[21,22], which speaks to the generality of the phenomenonand suggests new directions for research in microfluidics.ThefundamentaleffectofICEOataninert(non-electrode)metal surface has been predicted theoretically, but remainsto be demonstrated experimentally in a microfluidic device.Here,wepresentexperimentswhichrevealICEOconvectionrolls around an electrically isolated platinum wire in a poly-mer channel driven by an ac voltage. The setup is similar tothe canonical problem of a metal cylinder[19,20](or sphere [21])in a suddenly applied uniform field, shown inFig. 1, although the geometry is more complicated since the wirerests on one wall of the channel. We make detailed maps of the flow field inside the channel and compare with varioustheoreticalmodels,solvednumericallyforthespecificexper-imental geometry. Analogous experiments on metal colloidshave also been reported by Gamayunov et al.[23], but thefixed and simple geometry of a microfluidic channel allowsmore direct, quantitative testing of the theory, as well as newtechnological applications.
2. The experiment
2.1. Basic setup
As a simple first experiment to illustrate ICEO flow ata non-electrode metal surface in a microfluidic device, weconsidered the experimental setup shown inFig. 2. A plat-inum wire of circular cross-section was attached to the wallof a polymer microchannel containing low-concentrationKCl electrolyte. An ac voltage was applied from distantends of the channel (without any electrical connectionsto the wire) to produce an oscillating background electricfield transverse to the wire. The observed time-averagedICEO flow resembled that of Fig. 1(c), aside from geo- metrical corrections due to the channel walls, which weretaken into account in the theoretical models below. Theflow was visualized by tracking fluorescent tracer particles
Fig. 1. Induced-charge electro-osmosis in an electrolyte around a metal wire in a suddenly applied background electric field: (a) after the near-instantaneousrelaxation of electrons, the metal is an equipotential surface; (b) charging of the double layer by ionic fluxes expel the field lines, leaving a non-uniform(dipolar) charge distribution in the double layer around the metal; (c) non-linear (steady) electro-osmotic slip results as the tangential field acts on the induceddouble-layer charge.
J.A. Levitan et al. / Colloids and Surfaces A: Physicochem. Eng. Aspects 267 (2005) 122–132
Fig. 2. Schematic diagram of the experimental setup. A 100
m diameterand 1mm long platinum wire is attached to one side of a 200
m thick channel, which is 1mm deep and 1cm long. An ac voltage is applied acrossthelengthofchannel(fromlefttoright),transversetothewire,byelectrodes(not shown in the image) 1cm apart. The time-averaged ICEO flow is visu-alized by imaging fluorescent tracer particles in a horizontal slice slightlybelow the wire (dashed plane) using an inverted optical microscope.
through an inverted optical microscope in slices transverseto the wire, allowing quantitative comparisons with the basictheory.
2.2. Device fabrication
Molds for the microfluidic channels were made by spin-coatingnegativeresist(MicrochemSU-82050)onto4in.sil-icon wafers and patterned with high-resolution transparencymasks. The patterned resist layer was then hard-baked. Thetop layer of the device was cast as a thick layer of 5:1 A:BGE Silicones (GE Silicones, RTV 615) using the mastermold.Thelayerwascuredforapproximately40minat80
C.Ports were punched through this thick layer using 20gaugeluer stub adapters. The bottom layer of the device was 20:1A:B GE Silicones, spun-coat at 4000rpm onto a #1 glass24mm
C.Thetop layer was cleaned with isopropyl alcohol and dried withnitrogen. For additional details for soft-lithographic fabrica-tion of microchannels, the reader is referred to Refs.[24,25].The experimental channel was 200
m thick, 1mm deepand 1cm long as shown inFig. 2. The ac voltage was appliedacross the longest dimension of 1cm. The 1mm long sectionof 100
m diameter platinum wire was cut and cleaned inacetoneandisopropylalcoholandthenplacedinthecenterof thechannelonthetopsection.Thetopsectionwasthenplacedon the bottom layer and the assembled layers were curedfor an additional 1h at 80
C. Devices were also fabricatedusingDowCorningSylgard184withsimilarresults.Variousorientations of the platinum wire in the channel, for instance,laid vertically in the channel, were also achieved via thisprocess.
2.3. Flow generation and visualization
Tovisualizetheflow,small(500nm)fluorescentseedpar-ticles (G500, Duke Scientific, CA) with peak excitation andemission at 468 and 508nm, respectively, were loaded intothe microchannel at a volume loading fraction of 0.01%.The neutrally buoyant polystyrene spheres were suspendedin 1mM KCl solution (prepared from granular MalinckrodtAR KCl), which has a screening length of 
10nm. Thesolution was loaded into the channel with a syringe througha hollow metal fitting, which also served as the ground elec-trode.The open end of the channel was capped with a 1mmdiameter gold wire which served as the second electrodefor the oscillating voltage, applied across the channel us-ing a function generator (33220A, Agilent, Palo Alto, CA)connected through a power amplifier (Model 50/750, Trek,Medina, NY). This setup enabled the application of between0 and 750V with a maximum frequency of 3MHz, butthe experiments reported here were restricted to
100V at
500Hz. The typical electric field in the channel was thusin the range, 0–100V/cm, which corresponded to an approx-imate background voltage drop across the 100
m wire of 0–1V.Aninvertedmicroscope(Axiovert200M,KarlZeiss,Ger-many) was used to follow the tracer particles in the mi-crochannel. The illumination source was a broad spectrum100W mercury lamp (LEJ GmbH, Germany). The fluores-cent spheres were imaged through a cube filter consistingof a band-pass excitation filter (450–490nm), dichroic mir-ror with a cut-off wavelength of 510nm and a barrier long-pass emission filter (515nm). The 10
objective (numeri-cal aperture of 0.25) had a measurement depth of 28
m ascompared to the 200
m depth of the device[28].The im- ages were recorded onto a CCD camera (DFW-V500, Sony,Japan) with a 640pixel
480pixel array and 8-bit read-outresolution. The field of view corresponding to the CCD pixelsheet size and the magnification is 474
m in theobject plane.
2.4. Particle image velocimetry
Particle image velocimetry (PIV) is a non-intrusive opti-cal diagnostic technique which tracks displacements of col-lections of tracer particles to characterize flow fields[26].Micro-particle image velocimetry (
PIV) has been imple-mented to map velocity fields within microfluidic devices.
PIV utilizes fluorescent microscopy coupled with special-ized cross-correlation algorithms to yield vectors with mi-crometer spatial resolution[27].Fig. 3shows a representative raw image from the experi-ment. The background noise, mostly attributable to fluores-cent particles adsorbed to the platinum surface, is observedin this figure. Background subtraction was performed to re-move the fluorescence from the stuck particles and improvesignal-to-noiseratio(SNR).Imagesweresynchronouslycol-

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