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NUMERICAL STUDIES OF NONLINEAR KINETICS IN INDUCED-CHARGE ELECTRO-OSMOSIS Misha Marie Gregersen∗ , Martin Z. Bazant∗∗ , and Henrik Bruus∗ Department of Micro and Nanotechnology, Technical University of Denmark, DTU Building 345 East, DK-2800 Kongens Lyngby, Denmark ∗∗ Department of Mathematics, Massachusetts Institute of Technology, Cambridge, MA 02139, USA

∗ MIC-

Summary We present a numerical study of induced-charge electro-osmosis (ICEO) of electrolytes in microﬂuidic channels containing a ﬁxed dielectric structure. ICEO is the nonlinear electro-osmotic slip that occurs in the electrolyte when an applied electric ﬁeld acts on the ionic charge it induces around the polarizable surface of the dielectric structure. We also establish a method for optimizing the shape of the dielectric structure for any given objective function, e.g. the resulting pumping velocity achieved for asymmetric structures.

INTRODUCTION Induced-charge electro-osmosis (ICEO) is the nonlinear electro-osmotic slip that occurs in an electrolyte when an applied electric ﬁeld acts on the ionic charge it induces around an polarizable surface of any dielectric in contact with the electrolyte. Within the past few years in microﬂuidics, a number of cases of nonlinear ICEO ﬂows with both AC and DC forcing have been observed around isolated and inert (but polarizable) objects. Early examples of dielectric structures comprise ﬂat dielectric stripes on a planar blocking electrode [1], protruding dielectric corners far from any electrode [2], and channel junctions sustaining nearby electrokinetically driven vortices [3]. More recent examples of experimental ICEO observations involve symmetric microﬂuidic ICEO ﬂow [4], reduction of ICEO at high voltage bias in the nonlinear regime [5], and ICEO-based mixing in microﬂidc systems [6]. The ICEO ﬂows have also been studied theoretically, from analysis of the basic basic concept [7], over a thorough treatment of the general equations [8], to a more recent detailed analysis of symmetry breaking [9]. These experimental and theoretical studies suggest that a rich variety of nonlinear electrokinetic phenomena at polarizable surfaces remains to be exploited in microﬂuidic devices. The aim of this paper is to advance the understanding of ICEO by numerical simulation of the nonlinear governing equations of the electrokinetics of an electrolyte in a conﬁned microﬂuidic channel. We also establish a method for optimizing the shape of the dielectric structure for any given objective function, e.g. the resulting pumping velocity achieved for asymmetric structures. MODEL AND GOVERNING EQUATIONS We consider, as sketched in Fig. 1(a), an inﬁnite parallel-plate capacitor with conducting yz-planes at x = ±L kept at potentials ±φ0 . Somewhere in between the plates is placed a dielectric structure, and the rest of the space is ﬁlled with an electrolyte having a viscosity η, a constant density ρ, and containing concentrations c± of ions with charges ±Ze and mobilities β± . The whole system is translationally invariant along the z axis. The velocity and pressure ﬁelds of the electrolyte are denoted u and p, respectively, while the ionic current densities are denoted J± . The electric properties are described by the potential φ and the permittivity (r), which vary in space due to the presence of the dielectric structure. The governing equations of the system are modeled by the steady-state Navier–Stokes and continuity equation for incompressible ﬂuids, the Maxwell equation for the static potential, and the Nernst–Planck and continuity equation for the ions: ρ u· u=− p+η · u = 0, · φ = −Ze c+ − c− , J± = −β± · J± = 0. RESULTS The governing nonlinear, coupled partial differential equations have been implemented in the commercial software Comsol Multiphysics. A typical result for the resulting potential and ICEO ﬂow ﬁeld is shown in Fig. 1(b) and (d), respectively. The ﬂow ﬁeld shows a characteristic four-vortex structure also found in the analytical work by Bazant et al. [9]. However, as seen in Fig. 1(c) the agreement with the analytical result is only qualitative. The reason for the quantitative discrepancy is that here the fully nonlinear equations have been solved, and the system is in a conﬁned space, while the analytical result was obtained for an unbounded electrolyte in the limit of inﬁnitely thin Debye layers and in the linear, high-temperature Debye–Hückel limit. The advantage of our numerical method is that without the limiting approximations of the analytical ± c± φ+ kB T Ze + u c± ,

2

u − Ze c+ − c−

φ,

(1a) (1b) (1c)

c±

(1d) (1e)

(a)

φ [mV]

v p η ρ

2

J± β± c±

1 0

(b)

(d)

8 6 4

y [10−1 µm]

−1

2 0 −2 −4 −6 −8 −8 −6 −4 −2 0 2 x[10−1 µm] 4 6 8

−φ0 y x

1 2

φ0 φ

−2 1 0.5 y [µm]

v [10−1 µm/s]

0 −0.5

8 6 4 2 0 −8 −6 −4 −2 2 0 y[10−1 µm]

0.5 0 x[µm] −1 −1 −0.5

1

(c)

4

6

8

Figure 1. (a) A sketch of the model in the xy plane with the two parallel plate electrodes to the left and right, and the dielectric structure in the middle. All ﬁelds are mentioned. (b) A numerical simulation of the electric potential φ for a triangular dielectric structure; its shape is given by the conformal mapping eiθ + 0.4 e−i2θ of the unit circle. (c) A comparison of the numerically (red dashed line) and analytically (blue line) calculated ICEO ﬂow velocity |v| along the line with parallel to the y axis through x = −2.4 µm. (d) A numerical simulation of the ICEO ﬂow ﬁeld in the xy plane. The red line indicates the position of the line scan in panel (c).

approach, it can form the basis for a wider range of studies, such as optimization of the system design with respect to various quantities related to ICEO. In particular we aim at maximizing the nonzero ﬂowrate through the microﬂuidic channel that arises when the dielectric structure has spatial asymmetries. To optimize the ﬂowrate of the ICEO device we employ the method of topology optimization. This method has recently been adapted to microﬂuidcs and implemented in Comsol Multiphysics [10, 11]. The method relies on the introduction of an artiﬁcial porous medium in the ﬂuidic system. The porosity is characterized by a parameter ﬁeld γ(r) which takes values between zero, corresponding to small pores and high friction (a wall-like structure, here the dielectric structure), to unity, corresponding to large pores and low friction (pure liquid, here the electrolyte). The parameter ﬁeld couples to the governing equations through a Darcy friction force −α(γ(r))v added to the Navier–Stokes equation, and through the electric permittivity (γ(r)) and the mobilities β± (γ(r)). We have implemented γ-dependence of all three coefﬁcients such that we have zero Darcy friction as well as high permittivity and conductivity for γ being unity (the liquid phase), and large Darcy friction as well as low permittivity and conductivity for γ being zero (the dielectric phase). From an initially given γ0 (r), the governing equations are solved. The objective function, here the ﬂow rate, is calculated together with the so-called sensitivity of the system. From the latter an improved update of the parameter ﬁeld γ(r) is determined, and a new iteration is run. At some point the iteration converges, and in this state the parameter ﬁeld is either zero or unity in most of space; hardly no intermediate values are found. As a result regions with pure liquid and with the dielectric can be identiﬁed, and thus the optimal shape of the dielectric structure can be determined. CONCLUSIONS We have established a numerical method by using Comsol Multiphysics that allows us to calculate the ICEO ﬂow resulting from nonlinear kinetics in complex geometries, i.e. for arbitrarily shaped dielectric structures in microﬂuidic channels with electrolytes. We have introduced a continuous parameter ﬁeld γ(r), by which regions of pure electrolyte and of dielectric material can be identiﬁed and changed. One such calculation forms a single step in the iterative method of topology optimization. Using that it will be possible to explore the rich physics in the complex nonlinear ICEO ﬂows and in particular to ﬁnd optimized geometrical shapes of the dielectric to obtain maximal ICEO pumping. References

[1] Nadal F., Argoul F., Kestener P., Pouligny B., Ybert C., and Ajdari A.: Electrically induced ﬂows in the vicinity of a dielectric stripe on a conducting plane. Euro. Phys. J. E 9: 387–399, 2002. [2] Thamida S.K. and Chang H.C.: Nonlinear electrokinetic ejection and entrainment due to polarization at nearly insulated wedges. Phys. Fluids 14: 4315–4328, 2002. [3] Takhistov P., Duginova K., and Chang, H.C.: Electrokinetic mixing vortices due to electrolyte depletion at microchannel junctions. J. Colloid ˝ Interface Sci. 263: 133-U143, 2003. [4] Levitan J.A., Devasenathipathy S., Studer V., Ben Y., Thorsen T., Squires T.M., Bazant M.Z.: Experimental observation of induced-charge ˝ electro-osmosis around a metal wire in a microchannel. Colloids Surf. A 267: 122U-132, 2005. [5] Soni G., Squires T.M., and Meinhart C.D.: Nonlinear phenomena in induced-charge electroosmosis: a numerical and experimental investigation. Proc. MicroTAS 2007, 7–11 Ocober, Paris, France: 291–293, 2007. [6] , Harnett, C.K. and Kanouff, M.P.: ICEO-based microﬂuidic mixing. private communication, 2008. [7] Bazant M.Z. and Squires T.M.: Induced-Charge Electrokinetic Phenomena: Theory and Microﬂuidic Applications. Phys. Rev. Lett. 92: 066101 1–4, 2004. [8] Squires T.M. and Bazant M.Z.: Induced-charge electroosmosis. J. Fluid Mech. 509: 217–252, 2004. [9] Squires T.M. and Bazant M.Z.: Breaking symmetries in induced-charge electro-osmosis. J. Fluid Mech. 560:65-101, 2006. [10] Olesen L.H., Okkels F., and Bruus H.: A high-level programming-language implementation of topology optimization applied to steady-state Navier-Stokes ﬂow. Int. J. Numer. Meth. Eng. 65: 975–1001, 2006. [11] Okkels F and Bruus H: Scaling behavior of optimally structured catalytic microﬂuidic reactors. Phys. Rev. E 74: 017301 1–4, 2006.

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