PRL 96, 134505 (2006) PHYSICAL REVIEW LETTERS week ending 7 APRIL 2006 Selection of Two-Phase Flow Patterns at a Simple Junction in Microfluidic Devices W. Engl, K. Ohata, P. Guillot, A. Colin, and P. Panizza* Laboratoire du Futur, Rhodia/CNRS FRE 2177, 178 Avenue A. Schweitzer, 33608 Pessac, France (Received 18 January 2006; published 7 April 2006) We study the behavior of a confined stream made of two immiscible fluids when it reaches a T junction. Two flow patterns are witnessed: the stream is either directed in only one sidearm, yielding a preferential flow pathway for the dispersed phase, or splits between both. We show that the selection of these patterns is not triggered by the shape of the junction nor by capillary effects, but results from confinement. It can be anticipated in terms of the hydrodynamic properties of the flow. A simple model yielding universal behavior in terms of the relevant adimensional parameters of the problem is presented and discussed. DOI: 10.1103/PhysRevLett.96.134505 PACS numbers: 47.56.+r, 45.70.Qj, 47.61.Jd An important class of ‘‘out of equilibrium’’ patterns occurs by forcing immiscible fluids in interconnected thin gap networks, a phenomenon frequently encountered in nature as well as in many man-made systems [1,2]. Illustrative examples include the flows of hydrocarbons and water through porous rocks during oil recovery, parallel flows used for various microfluidic applications [3], as well as flow of air in the lungs. These fluid-fluid displacements generate preferential flow pathways along one of the fluid flows, forming patterns ranging from compact to ramified and fractal [4]. The formation and selection of these patterns are challenging problems in the field of nonequilibrium physics [5] and central for many industrial applications. For instance ‘‘tongues of water in oil’’ is a limiting factor in secondary oil recovery. One of the major difficulties in achieving a good understanding of preferential pathways in interconnected networks is the large number of parameters potentially involved. These include the viscosity of the two fluids, their respective flow rates, the surface tension between them, as well as the topology of the network [6]. The aim of this Letter is to address an essential element of immiscible flows in porous media or branched networks, which is the effect of a bifurcation where the flow is separated into two streams. We focus on the simplest configuration, namely, a T junction. As sketched in Fig. 1, our goal is to understand how a laminar stream and its carrier phase divide between these two branches. We start by reporting experiments which show the existence of two possible hydrodynamic regimes: the stream is either directed in only one of the arms, yielding a preferential flow path for the dispersed phase, or splits between both. Surprisingly, the mechanism at work in this phenomenon is not triggered by the shape of the junction nor by capillary effects but results from the 3D structure of the confined stream. A simple hydrodynamic model yielding universal behavior in terms of the different adimensional parameters of the problem is presented and confronted with our experimental data. Experiments are performed in microchannels, fabricated into poly(dimethylsiloxane) (PDMS) transparent elasto0031-9007=06=96(13)=134505(4)$23.00 mers, using classical soft lithography techniques. The microfluidic devices are prepared by placing a PDMS slab with the following channel features, height h 20 m and width d 100 m, onto either a glass cover slip or a flat PDMS slab. For each device, laminar streams are formed at a symmetrical cross flow junction (Fig. 1). The two Newtonian immiscible fluids used in our experiments are millipore water and silicone oil (Fluka), whose respective viscosities at T 20 C are w 1 mPa s and o 20 mPa s. Using separate syringe pumps, the flow rates of these two fluids are independently controlled and adjusted in order to form a water in oil (W-O) stream. For both fluids, the Reynolds numbers can be estimated using Re Qf f =hf , where Qf , f , and f are, respectively, the fluid flow rate and its mass volume and viscosity. The values obtained for our experiments are smaller than 0.25 indicating that flows are laminar. To study the behavior of the laminar stream at a junction, we work with the microfluidic analogs of electric current splitting devices [7] (Fig. 1). Briefly, the stream is directed towards a T junction, referred from now on as the inlet T junction. In order to achieve the same pressure drop in both side arms, the two arms merge at another T junction, referred as to the outlet junction (see Fig. 1). As shown later on, by adjusting the relative lengths L1 and L2 of the two sidearm channels it is possible to control the behavior of the jet in the device. FIG. 1. Schematic representations of the experimental setup. 134505-1 © 2006 The American Physical Society PRL 96, 134505 (2006) PHYSICAL REVIEW LETTERS Images of the flows are captured and recorded using an inverted microscope equipped with a CCD camera. Experiments are performed by fixing the value of the water flow rate (Qw 600 l=h), while varying that of the oil (Qo ). Figure 2 shows the evolution of the stream at the inlet T junction as a function of q Qo =Qw , for LL21 1:75 and for different shapes of the junction. For small values of q, the stream splits at the junction, forming two secondary coflows in each sidearm. At the outlet T junction, these two coflows merge to reform the initial stream. As shown on Fig. 2, the asymmetry between the two secondary coflows becomes more and more important as q increases. When q is slightly increased above a critical value, qc 0:13, an unexpected and surprising phenomenon occurs: the initial stream no longer splits at the inlet T junction, but instead deviates towards the shorter sidearm. In this flow regime, the junction therefore acts as a perfect filter, since water is no longer flowing in the longest arm. In the shortest arm, a coflow configuration is witnessed since the deviated stream is in contact with one of the two channel vertical edges. At a critical value of q, it suddenly loses contact with this edge. The position of the stream in the shortest outlet then becomes more and more central upon increasing the value of q. The (S-F) transition between splitting and filtering is independent of the angle between the three arms of the junction (Fig. 2). In addition, it persists if the flat PDMS cover slab is replaced by a glass cover slip or if, , the surface tension between oil and water is varied (as later shown on Fig. 5), indicating that the physical mechanism at play in this phenomenon is not likely triggered by wetting properties. To elucidate the origin of this phenomenon, we first characterize the three-dimensional structure of the flow using confocal microscopy experiments. A minute amount of rhodamine (Fluka) is added to the aqueous phase. Figure 2 displays a 3D image of the flow, obtained by reconstruction from several juxtaposed horizontal sections. For channel features (h d), we observe a quite unexpected result since the water stream is not wrapped by an week ending 7 APRIL 2006 oil film but instead wets both the top and bottom surfaces of the channel, independently of their chemical nature (glass or PDMS). At first sight, this result is very striking considering that the wettability affinity for PDMS is much stronger for silicone oil than for water and that the capillary numbers at play in our experiments are very low (typically smaller than 102 ). This counterintuitive phenomenon results from confinement [8]. Briefly, a laminar stream flowing along a constant cross section channel must present the same constant curvature shape in any perpendicular cross section of the channel. For a given set Qo ; Qw and a given channel shape, only one value of the stream curvature, c, exists. This value depends on o =w , q, and . Under certain experimental conditions [8], c1 may eventually be larger than h, leading to truncated cylindrical streams being then in contact with the two horizontal channel surfaces. This situation is favored when the channel features are very anisotropic (h d) and q and are small. Two parameters are then necessary to describe the stream: its width w and c, the curvature of the W-O interface. When w=h > 1, w depends only on and q at first order (the wetting properties of the two fluids and their affinity for the substrate imposes c, but have second order effects on w). This coincides with our experimental observations. Now that the structure of the flow is well established, the S-F transition can be understood only using hydrodynamic considerations. Let us start with Stokes equations and incompressible flows for both fluids with no slip boundary conditions. In view of experimental results, reasonable assumptions are to neglect the geometry details of the inlet T junction, namely, the influence of the angle between the three arms of the inlet T junction, to consider that the water stream wets both top and bottom surfaces and that the interface between both phases can be well approximated by a plane [Fig. 3(b)]. Within this framework, let us first analyze the hydrodynamic configuration where the stream splits at the inlet junction (Fig. 3). First, look at a steady state coflow in a straight channel of constant cross section S h d and length L. For a given position of the interface between the water and the FIG. 2. Behavior of the stream at the inlet junction for different values of q (given in the images) and o 20 mPa s. 134505-2 L2 L1 x2 features. Since the water stream wets both the top and the bottom channel surfaces, no exchange of oil between the two sides of the incoming stream is possible at the inlet junction. It therefore follows that for a symmetric oil injection (Fig. 1) the oil flow rates must be equal in both sidearms of the junction (Fig. 3). For i 1; 2, such a condition writes Pfh; d 1 Qo (5) G 1 Xi ; : Li o 2 x1 h o w o d x2 Q0/2 x1 Q0/2 h d FIG. 3 (color online). (a) 3D reconstructed confocal image for a splitting flow pattern and (b) its schematic representation. oil domains, X dx , the velocity profiles of both fluids and therefore their respective flow rates can be numerically computed using a finite discretization of the Stokes equations. The computations are performed with the scientific software SCILAB, developed by INRIA (France). A rapid analysis shows that the expressions of the two flow rates follow Pfh; d GX; Lw (1) Pfh; d 1 G 1 X; ; Lo (2) Qw and Qo week ending 7 APRIL 2006 PHYSICAL REVIEW LETTERS PRL 96, 134505 (2006) By dividing Eqs. (3) and (4) by Eq. (5), a system of two nonlinear equations between only X1 and X2 and the three experimental parameters , , and q is obtained, yielding the existence of universal behaviors . To test this, we first compute the variations of X1 and X2 from this set of equations as a function of q for 1:75 and 20 and compare them to our experimental data. As shown on Fig. 4, all experimental data obtained for different water and oil flow rates fall on the master curve predicted by the model. Above a critical value qc 0:14, all the solutions admit X2 0, indicating that for q > qc the stream can no longer split at the inlet T junction and therefore all the dispersed phase must flow through the shortest channel. This is the filter regime. Another test is to compare numerical results to experimental results when q and are fixed but when is allowed to vary (see Fig. 5). To do so, experiments are now performed at 1:75 using water and silicone oils of different viscosities. As before, we set Qw and change Qo . In agreement with our numerical results, we observe that the S-F transition strongly depends on when q and are fixed (Fig. 5). As expected by the model, a universal behavior is observed by plotting X2 as a function of q (inset of Fig. 5). The value of the critical flow rate ratio X1 /d 1 1 Qw Qo Pfh; d GX1 ; GX2 ; ; L2 w Pfh;d 1 1 : G 1 X1 ; G 1 X2 ; L2 o (3) (4) The third equation results from the unexpected shape of the incoming stream (Fig. 3) observed for our channel 0.8 0.6 0.8 0.4 X2/d where fh; d and GX; are two functions having, respectively, m4 and no units, and P the pressure drop between the two extremities of the channel. For the branched network of (Fig. 1), three variables are necessary to describe a flow situation where the stream splits at the junction, namely, the positions of the water-oil interfaces in each side arms X1 and X2 and P, the pressure drop between the inlet and outlet T junctions. On this basis, three relations are necessary to solve this problem. Two predictable equations are obtained from the conservations of the water and the oil flow rates at the junction: 0.6 0.2 0.4 0 -3 10 10 -2 10 -1 10 0q 0.2 0 10 -3 10 -2 10 -1 10 0 10 1 q FIG. 4. Positions of the W-O interface in the longest side arm (and in the shortest arm for the inset) as a function of q. The two fluids are water and silicone oil (o 20 mPa s). The water flow rate is fixed, and the oil flow rate varied. The (䊐), (4), (), and (5) symbols correspond to experiments performed, respectively, at Qw 200, Qw 300, Qw 400, and Qw 600 l=h with a junction angle of 90. The solid symbols correspond to experiments performed at Qw 600 l=h but with junction angle 45 (䉬) and 135 (䊉). The continuous and dashed lines correspond to the numerical solutions of the model. 134505-3 1 1 2 10 X2/d 0.8 0.8 X2/d week ending 7 APRIL 2006 PHYSICAL REVIEW LETTERS PRL 96, 134505 (2006) 0.6 0.4 0.6 0.2 0.4 0 -2 10 -1 10 0 10 qη η 1 10 1 10 0.2 0 10 -3 10 -2 10 -1 10 0 10 1 q 0 10 FIG. 5. Positions of the W-O interface in the longest sidearm as a function of q for different values of . (), (䉱), and (5) symbols correspond to experiments performed with different silicone oils ( 0:043 N m1 ) having respective viscosity numbers: 20, 50, and 100, for Qw 600 l=h. (䊉) correspond to an experiment performed with hexadecane: 0:052 N m1 and 3, for Qw 200 l=h. The continuous lines are the numerical solutions of the model. above which the filter regime exists is then given by qc 2:9. To test the influence of the last adimensional parameter, on the S-F transition, we set a value for the product q and compute X2 as a function of . A systematic numerical study reveals that, for any values of q, solutions of the set of equations present a X2 0 domain when becomes larger than a critical value c , satisfying c 1 2:15=q (Fig. 6). To check this prediction, we have fabricated several microfluidic devices having the same channel cross but different values of . For each device, experiments are performed with water and silicone oil (o 20 mPa s) by changing the values of q (we set Qw and change Qo ). Under these conditions, we observe that the value of qc , characterizing the S-F transition decreases when increases. Consequently, as predicted by the model, if the value of the product q is fixed, a S-F transition can therefore be witnessed by merely increasing the value of (inset of Fig. 6). In summary, the features of the S-F transition are well captured by our simple hydrodynamic model. The origin of this phenomenon lies in the absence of oil exchange between the two sides of the incoming stream due to its strong confinement. This effect can therefore be witnessed whether the injection of an oil stream is symmetric (see Fig. 1) or not. For a symmetric injection of oil, the universality of this phenomenon can be summarized by a diagram which maps the nature of the selected flow pattern as a function of the two relevant adimensional numbers of the problem: q and (Fig. 6). Such a general effect opens up a way to digital and integrated microfluidic devices. Thus, the (S-F) transition occurring at the inlet T junction operates either as a flow rate or as a viscosity comparator [9] 10 filter regime splitting regime -1 0 10 1 λ -1 10 FIG. 6. Universal diagram mapping the nature of selected flow pattern: filter or splitting as a function of the two pertinent adimensional parameters of the problem. The continuous line, q 2:15 11 , is the transition line between the two flow regime predicted by the model, whereas () symbols corresponds to experimental data. Inset: flow patterns observed at the junction for (a) 1:25, (b) 2, and (c) 5 when 20 and q 0:05. depending on which adimensional variable, or q, is known. Since the initial stream reforms at the outlet T junction, such comparator elements whose threshold values are fixed by can be integrated into cascade to design inexpensive digital microfluidic devices. In its simplest version, a succession of comparators with different values of simply obtains an estimation of a fluid viscosity. Along this line, work is in progress to develop a continuous measurement device. *Electronic address: pascal.panizza-exterieur@eu. rhodia.com [1] Shape and Structure: From Engineering to Nature, edited by A. Bajan (Cambridge University Press, Cambridge, England, 2000). [2] Porous Media: Fluid Transport and Pore Structure, edited by A. Scheidegger (University of Toronto, Toronto, 1974). [3] J. Knight, Nature (London) 418, 474 (2002). [4] M. Cieplak and M. O. Robbins, Phys. Rev. Lett. 60, 2042 (1988). [5] J. S. Langer, Rev. Mod. Phys. 52, 1 (1980). [6] J. P. Stokes, D. A. Weitz, J. P. Gollub, A. Dougherty, M. O. Robbins, P. M. Chaikin, and H. M. Lindsay, Phys. 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