Professional Documents
Culture Documents
Articles
Laboratoire de Physico-Chimie The orique, UMR 7083 CNRS-ESPCI, 10 rue Vauquelin, F-75231 Paris France,
LPN-CNRS, Route de Nozay, Marcoussis 91460 France, and Division of Engineering and Applied Sciences,
Harvard University, Cambridge, Massachusetts 02138
We highlight the fact that hydrodynamic dispersion in depart notably from the circular capillary usually described in
shallow microchannels is in most cases controlled by the textbooks. As a consequence, many analyses refer to situations
width of the cross section rather than by the much thinner with only one transverse dimension (radius or height), a procedure
height of the channel. We identify the relevant time scales that we will show can lead to order of magnitude errors in the
that separate the various regimes involved. Using the estimation of dispersion. In principle, the basic procedure for
lubrication approximation, we provide simple formulas properly quantifying mass transport in laminar pressure-driven
that permit a quantitative evaluation of dispersion for most flows is well established, and follows the seminal works of Taylor2
shallow cross-sectional shapes in the long-time Taylor and Aris;3 see also Brenner and Edwards.4 Either of the two
regime, which is effectively diffusive. Because of its approaches, though somewhat different in detail, allows one to
relevance for microfluidic systems, we also provide results quantify the dispersion for arbitrary channel cross sections. In
for the short-time ballistic regime (for specific initial one recent application, Dutta and Leighton5 discussed how to limit
conditions). The special cases of parabolic and quasi- dispersion in pressure-driven flows by tailoring the cross-sectional
rectangular shapes are considered due to their frequent shape of the microchannel. For simple shapes of the channel cross
use in microsystems. section (e.g., two planes, a circle, and an ellipse), analytical results
for dispersion are available, while more complicated shapes
Hydrodynamic dispersion refers to the inevitable spreading require numerical analysis (see also ref 6).
along the flow direction of dissolved or suspended Brownian In this paper, we provide basic results for describing simply
particles in a flowing fluid, the ultimate origin of the spreading and quantitatively the effect of hydrodynamic dispersion for
being related to velocity variations in the direction transverse to situations where the microfluidic channel has a slender, shallow
the mean flow. The effect is particularly significant in laminar flows cross section with a typical height h0 much smaller than the width
in channels for which there is generally a gradual change in w (see Figure 1, top). These situations are numerous in micro-
velocity from zero at the boundary to a maximum value in the fluidic devices, partly as a consequence of the various microfab-
center. The dispersion significantly reduces the resolution of rication methods (see, for example, ref 7 and references therein).
analytic studies performed using pressure-driven flow in micro- Some common cross sections include quasi-rectangular and
fluidic devices and analytical lab-on-a-chip systems (ref 1 and trapezoidal shapes (e.g., via chemical etching of crystalline silica),
references therein). Such analytic studies include, for example, quasi-parabolic shapes (e.g., PDMS channels used in multilayer
separating species or determining rates of chemical reactions. devices), etc.
Hydrodynamic dispersion also limits the number of samples that There are two main contributions in this paper. First, we
can be transported sequentially in a given microchannel and demonstrate and emphasize that, when h0 , w, in almost all cases
thereby limits the throughput of the device. (i.e., we exclude quasi-rectangular cross sections) hydrodynamic
Although such (Taylor) dispersion is considered a well- dispersion is controlled by the width w, the larger of the two
understood phenomenon, it nevertheless remains difficult to transverse dimensions, and not by the height h0 of the micro-
quantify in practice for many microchannel configurations, which channel. This fact is in contrast with calculations of the hydro-
* To whom correspondence should be addressed. E-mail: armand@ (2) Taylor, G. I. Proc. R. Soc., London Ser. A 1953, 219, 186.
turner.pct.espci.fr. (3) Aris, R. Proc. R. Soc. A 1956, 235, 67-77.
Laboratoire de Physico-Chimie The
orique. (4) Brenner, H.; Edwards, D. A. Macrotransport Processes; Butterworth-Heine-
LPN-CNRS.
mann: Boston, MA, 1993.
Harvard University.
(5) Dutta, D,; Leighton, D. T. Anal. Chem. 2001, 73, 504-513.
(1) Stone, H. A.; Stroock, A. D.; Ajdari, A. Ann. Rev. Fluid Mech. 2004, 36, (6) Smith, R. J. Fluid Mech. 1990, 214, 211-228.
381-411. (7) Tabeling P. Introduction a` la microfluidique; Paris, 2003.
10.1021/ac0508651 CCC: $33.50 2006 American Chemical Society Analytical Chemistry, Vol. 78, No. 2, January 15, 2006 387
Published on Web 12/06/2005
the specific shape of the cross section by writing h(x) )
h0H(x/(w/2)), where H(X) is a dimensionless function that is zero
for X ) (1 and has a maximum equal to 1 between these two
points. We denote by S the constant cross-sectional area,
w/2
S ) -w/2 h(x) dx. We present results valid for the conditions
h0 , w , L, which are generally true for a large number of micro-
fluidic applications.
Flow and Transport of Particles. We assume that there is a
steady incompressible pressure-driven laminar flow in the channel.
The velocity field is directed along the channel axis, u ) u(x, y)ez,
and this field is independent of z so long as the cross-sectional
shape of the channel is constant. The cross-sectionally averaged
(mean) velocity V is defined as
z { }
For the sake of clarity, the paper is organized with the main
results clearly identified and mathematical details relegated to the
n w/2
-w/2 h(x)
0 c(x, y, z, t) dy dx dz
z (t) )
n
(3)
appendix. In the following section, we introduce the nomenclature
used, comment on the physical ingredients of the problem, and
w/2
-w/2 h(x)
0 c(x, y, z, t) dy dx dz
( I1
) ]
2
1
1
1 X
l ) -1 -1
H2(X) - 1 H(X) dX dX (7)
4I1 H(X) I3
Dlong 2
eff ) D(1 + lPew ) (9)
short times, larger that O(h02/D) but less than O(w2/D), during
which solute, having equilibrated in the short dimension starts
to sample the longer transverse dimension, and eventually a long We emphasize that remarkably the channel height h0 is
time regime, i.e., times longer than O(w2/D). If the thickness of completely absent in this long-time limit obtained for a smooth
the channel varies progressively along the largest transverse cross section (again abrupt shape changes, such as almost
dimension, then the thickness-averaged velocities will vary notice- rectangular shapes are not included in this analysis).
ably from place to place (i.e., at different positions x along the Dispersion at Shorter Times. Due to its special relevance
width). These variations induce a hydrodynamic stretching for microfluidic systems, we also investigate dispersion at shorter
extending throughout the short-time regime that adds up to the times, although the results are then not universal and depend on
one corresponding to velocity heterogeneities in the thickness the initial distribution of solutes.
(Figure 2). Only in the long-time regime can molecular diffusion Of special interest is the short time regime, i.e., times scales
progressively reduce this ballistic hydrodynamic spreading by longer than the (fast) time scale for molecular diffusion in the y
averaging throughout the cross section. direction but shorter than for that along the width of the channel;
The reason the transverse variations of velocities along the i.e., O(h02/D) < t < O(w2/D). Then, differences along the width
width dominate the overall Taylor dispersivity is because the x of the height-averaged velocities lead to an effective diffusion
statistical averaging is poorer in that direction due to the longer coefficient increasing linearly in time. For initial distributions
diffusion time required. For a quasi-rectangular channel, there is homogeneous along x, we explicitly obtain as described in the
little or no such transverse heterogeneity along the x direction of Appendix
( )
the height-averaged velocity (except for the vicinity of the side 1 d 2 Dt
walls), so that this source of dispersion is weak or absent. Dshort
eff (t) ) (t) = D + sV2t ) D 1 + sPew2 2
2 dt short w
Main Results. To substantiate these qualitative statements,
(10)
we now provide our analytical results, obtained, as detailed in the
Appendix, by combining the method of moments applied to
shallow channels as described in Aris3 with a lubrication descrip- where s is a dimensionless number that depends only on the
tion of the flow field. Our results thus hold for smooth shallow nondimensional shape H of the cross section:
cross-sectional shapes. The case of abrupt shape changes, as
occurs for nearly rectangular shapes, is discussed in the section s ) I1I5/I32 - 1 (11)
entitled Long-Time Dispersion for Quasi-Rectangular Shapes.
Long-Time Dispersivity. At long times, i.e., longer than
Again, h0 does not enter the description.
O(w2/D), the spreading of the sample is effectively diffusive
For even shorter times, i.e., shorter than O(h02/D), and for an
(Taylor-Aris dispersion). The average position is zeVt and the
initial distribution homogeneous in the cross section, a simple
variance, 2long, grows linearly in time
calculation using the lubrication description of the flow ( eq 25 in
2long(t) = (z - Vt)2(t) = 2D(1 + lPew2)t (5) the Appendix) yields a diffusivity formally similar to (10), with s
replaced by vs ) (6I1I5/5I32) - 1 ) s + (I1I5/5I32).
Crossover Time. A useful outcome of the previous analysis
where Pew is the Peclet number defined using the width w as the is an estimate for the typical crossover time txo between hydro-
relevant length scale (not h0) and V as the mean velocity: dynamic stretching and broadening by Taylor-Aris dispersion.
Analytical Chemistry, Vol. 78, No. 2, January 15, 2006 389
For large Peclet numbers (Pew . 1), equating the variance in the is characterized by the constant s ) (53/297) 0.178, so that
two regimes yieldsThis time scale, which as expected scales as the crossover coefficient (eq 12) from ballistic short-time to
diffusive long-time dispersion is xo ) (2l/s) ) (3347/96460)
2l w2 w2
txo = ) xo (12) 0.035.
s D D One application of these ideas is to the quantitative description
of the rotary mixer introduced by Quake and colleagues.9 This
device is commonly used to mix materials in one step of their
the time to diffuse the width, sets the limit of validity of the long-
processing in integrated systems using two-layer soft lithography.
time dispersive regime (eqs 6-10). Once again the channel width
For such systems, the operation of active elements such as valves
w is the important length scale.
is favored by using smooth rounded cross sections, and fabrication
In the above quantitative characterization of the dispersion
often results in parabolic cross-sectional shapes of the channels.
process, three shape-dependent dimensionless numbers, l, s, and
A typical microfluidic rotary mixer has a centerline radius R )
xo, have been introduced. We calculate and tabulate these
1000 m, width w ) 100 m, height h0 ) 10 m, and mean velocity
numbers for several representative shapes in the next section.
V ) 0.1 cm/s. Therefore, if we take the molecular diffusivity to
be D 5 10-6 cm2/s, then the crossover time for an experiment
DISCUSSION
General Remarks. As is well known in the literature on is typically txo 0.035w2/D 0.7 s. This time scale should be
hydrodynamic dispersion, the flow contributes a long-time effective compared with the average circulation time around the rotary
diffusion that varies as the square of the average velocity. mixer 2R/V 6 s. Thus, well before a single revolution, the
However, the channel dimension that enters the description is transport process is characterized by the description of dispersion
the width, not the height (assuming h0 , w), a fact that is based on the channel width. Our formulas can thus be used to
generally obscured since most analyses concern effectively two- refine the analysis presented by Squires and Quake,10 where only
dimensional situations. Furthermore, it is the square of that one dimension was considered, and provides guidance for a
dimension that enters the expression of the long-time Taylor complete 3D analysis of the problem along the lines of the 2D
dispersion, so that we are actually arguing that, for channels of analysis presented by Gleeson et al.11
aspect ratio, w/h0, of order 10, hydrodynamic dispersion is 100 Other Simple Shapes. We have also computed the values of
times larger than an analysis based on the height would suggest! the nondimensional parameters l, s, and xo ) 2l/s for elliptical
It is nevertheless worth noting that if the pressure drop p is and triangular cross sections, which are reported alongside those
specified for a channel of length L, then the mean velocity V ) for the parabola in Table 1. The long-time result for the elliptical
(h02I3p/12I1L), where is the viscosity of the fluid; this feature shape matches the limit of Ariss exact calculation (p 76 in ref 3).
brings the smallest dimension, the height, into the overall Focusing on the long-time dispersivity, two facts are im-
description. mediately apparent and worth emphasizing. First, as is common
The formulas above have been established using the lubrica- in such dispersion problems, the numbers are small for prefactors
tion approximation (see Appendix), so that we expect them to in a scaling theory, i.e., typically of order 10-3-10-2. Second, they
hold for arbitrary smooth and narrow cross sections. Note that are smaller (and so is dispersion) for flatter shapes, as is obvious
although the examples quoted here mostly refer to the format following the sequence triangle f parabola f ellipse. This result
common in microfluidics where one of the surface is flat (as corresponds to more uniform values of the velocity distribution,
described in Figure 1a), our results equally hold for any smooth i.e., smaller gradients of the height-averaged velocities.
narrow shape where the local height is ymax(x) - ymin(x) ) h(x). An extension of the above argument suggests making a
Also, the scaling forms are explicit in the formulas given above, connection to the case of the flattest shapes, i.e., rectangular
so that we now turn to the computation of the numerical shapes, for which exact (numerical) results are available. Blindly
coefficients for a set of representative shapes. applying the above results with h(x) ) h0 leads to numerical values
Parabolic Cross-Sectional Shapes. Parabolic cross sections that are exactly zero for both the short- and long-time coefficients,
are commonly found in many microfluidic geometries based on as the height-averaged velocity is uniform. This result is at odds
soft lithography techniques (e.g., ref 8). Thus, we provide explicit with existing calculations, but is logical in the framework of our
results for such shapes by using the formulas of the previous approximations as we explain in the next subsection.
section with h(x) ) h0(1 - (x/w/2)2) or H(X) ) 1 - X2. It is Long-Time Dispersion for Quasi-Rectangular Shapes. To
straightforward to evaluate the integrals in (7) to obtain establish the connection between our analysis for smooth shapes
and the rectangle (which is not smooth as h(x) goes abruptly from
3347 h0 to 0 on the two sides), we consider dispersion in quasi-
l ) 3.1 10-3 (13)
1081080 rectangular channels (Figure 3, top), which are flat for |x| <
w/2 - and then monotonically tend to zero over the length .
In addition to providing a connection to the case of a rectangle,
This value can immediately be compared with the more familiar
the topic is of interest on its own, as this kind of channel shape
(1/4)(1/48) 0.005 for the well-known prefactor of the disper-
is indeed found in some microfluidic systems.7 We start by general
sivity for pressure-driven flows in a circular tube (the (1/4) factor
stems from the comparison being made using the tube diameter, (9) Chou, H. P.; Unger, M. A.; Quake, S. R. Biomed. Microdevices 2001, 3,
rather than the radius, in place of w). The short-time dispersivity 323-330.
(10) Squires, T. M.; Quake, S. R. Rev. Mod. Phys. In press.
(8) Unger, M. A.; Chou, H. P.; Thorsen, T.; Scherer, A.; Quake, S. R. Science (11) Gleeson J. P.; Roche O. M.; West J.; Gelb A. SIAM J. Appl. Math. 2004,
2000, 288, 113-116. 64, 1294-1310.
1
{
H(X) ) 1 - |X|
for 0 e |X| e 1 -
for 1 - e |X| e 1
(15)
Here we have assumed, as sketched in Figure 1, the most where the constants In are defined in eq 8.
common situation in microfluidics, which is that the channel is (ii) Long-time regime: Then we introduce the intermediate
closed on one side by a flat plate so that the channel boundaries function
are at y ) 0 and y ) h(x). Any other smooth shape described by
ymin(x) and ymax(x) with ymax(x) - ymin(x) ) h(x) leads to identical
x
results in the present frame of approximations.
g(x) ) -w/2
j (x) - V)
dxh(x)(u (26)
The evolution equation for jc(x, z, t), which is adequate to
describe evolution at time scales longer than h02/D, is
to obtain from eqs 23 and 24, through an integration by parts (note
cj cj 2jc D cj
t
+u
j
z
)D 2+
h(x) x
h(x)
x ( ) (19) that g(( w/2) ) 0),
( )
z
d dx[g (x)/h(x)]
2
( )
that limit, given the normalization chosen c0(x, t) is a constant in
c0 1 c0
)D h (21) space and time c0(x, t) ) (dxh(x))-1, and c1(x, t ) 0) ) 0 if the
t h(x) x x origin of the z axis is chosen at the initial location of the center of
( )
c1 mass of the distribution dzf (z) ) 0. Then for times shorter than
1 c1
) (u
j (x) - V)c0(x, t) + D h (22) the diffusion time across the channel t < O(w2/D), it is clear that
t h(x) x x
we have the simple approximation c1(x, t) = (dx h(x))-1(uj (x) -
V)t. Thus, the evolution of the variance follows from eq 23:
with (cn/x) (x ) ( w/2, t) ) 0. The variance 2(t) )
(z - Vt)2(t) ) dxh(x)c2(x, t) evolves as
d dx h(x)(uj (x) - V) 2
(z - Vt)2 ) 2D + 2 t (28)
d
dt
(z - Vt)2 ) 2D + 2 dxh(x)(u
j (x) - V)c1(x, t) (23) dt
dx h(x)
Whatever the initial conditions, as time goes on, c0(x, t) tends Inserting the flow field in the lubrication approximation 25 yields
toward a constant value c0(t f ) ) c0 ) (dx h(x))-1, and the short-time result quoted in the text.
consequently, c1(x, t) tends toward a steady profile c1(x, t f ) )
c1 (x) given by This result can be used in (23) to compute the
( )
Received for review May 18, 2005. Accepted October 18,
d dc1 2005.
D h(x) ) - c0 h(x) (u
j (x) - V) (24)
dx dx AC0508651