Proceedings of the 4th European Conference on Microfluidics - Microfluidics 2014 - Limerick, December 10-12, 2014

µFLU14-92

ROLE OF DIFFUSION ON MOLECULAR TAGGING VELOCIMETRY

TECHNIQUE FOR RAREFIED GAS FLOW ANALYSIS
Aldo FREZZOTTI2, Hacene SI HADJ MOHAND1*, Christine BARROT1, Stéphane COLIN1
1
Université de Toulouse, Institut Clément Ader, Toulouse, France
sihadjmo@insa-toulouse.fr, christine.barrot@insa-toulouse.fr, stephane.colin@insa-toulouse.fr
2
Dipartimento di Scienze & Tecnologie Aerospaziali, Politecnico di Milano, Italy
aldo.frezzotti@polimi.it

KEY WORDS
Gas microflow, MTV, molecular tagging, DSMC, rarefied flow, diffusion equation

ABSTRACT
The Molecular Tagging Velocimetry (MTV) is a well-suited technique for velocity field measurement in rarefied gas flows.
Typically, a line is tagged by a laser beam within the gas flow seeded with luminescent acetone molecules. Positions of
the luminescent molecules are then observed at two successive times and the velocity field is deduced from the analysis
of the tagged line displacement and deformation. However, this displacement is affected by molecular diffusion, and
consequently, there is not a direct and simple relationship between the velocity field and the measured displacement of
the initial tagged line. In this paper, the role of the tracer molecules diffusion is investigated using the Direct Simulation
Monte Carlo (DSMC) method. The simulations demonstrate that the diffusion of these molecules closely depends on the
flow regime, and becomes significant as the degree of rarefaction of the gas flow increases. A simple reconstruction
algorithm based on the advection-diffusion equation has been developed to obtain the velocity profile form the
displacement field. This reconstruction algorithm has been numerically tested on DSMC generated data. It is shown that
the reconstruction becomes less effective as the degree of gas flow rarefaction increases. As expected, DSMC tests
demonstrate that the reconstruction error is reduced as the binary diffusion coefficient decreases.

1. INTRODUCTION
A number of microfluidic applications involve gas microflows in the slip flow regime [12], characterized by a
velocity slip and a temperature jump at the wall. Various models have been proposed in the literature [3, 12].
Experimental data, however, mainly concern flowrate measurements [9]. Local information on velocity fields
is nevertheless necessary to improve the discussion on theoretical models for slip boundary conditions. For
this goal, MTV could be a well-suited technique that could avoid some difficulties associated to the more
classic Particle Image Velocimetry (PIV) technique [10]. MTV uses seeding gas molecules, such as acetone,
which become luminescent once excited with a UV light. The region tagged by a UV laser beam is observed
at two successive times – the first time can correspond to fluorescence signal and the second one to
phosphorescence signal – and the velocity field is deduced from the displacement and deformation analysis of
the tagged region [8]. The spatial resolution, however, is constrained by the laser beam diameter, with a typical
minimum value of the order of 30 μm, which requires operating in channels with a hydraulic diameter around
1 mm. For this reason, microflows in the slip flow regime should be analyzed with Knudsen similitude,
reducing the pressure in order to reach Knudsen numbers in the range [10-3 –10-1], corresponding to this regime.
Gas flows in rectangular channels with high or moderate aspect ratios can be analyzed by one dimensional
molecular tagging velocimetry (1D MTV); in this case a single line or a series of lines are tagged
perpendicularly to the flow direction. The component of the displacement is then obtained in the direction of
the flow (Figure 1). 1D MTV has limitations compared with 2D MTV and stereoscopic (3D) MTV, but its

*
Corresponding author

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advantages are a simpler implementation and a higher spatial resolution in the vicinity of the wall [6]. This
makes 1D MTV a very promising technique for capturing velocity slip at the wall observed in rarefied regimes.
Preliminary velocity profiles were previously measured at atmospheric pressure, i.e. in the continuum flow
regime [10]. However, the displacement of tagged molecules is subject to molecular diffusion and at low
pressures corresponding to the slip flow regime in millimetric channels, typically in the pressure range [10-103
Pa], diffusion effects become significant and should be taken into account in the data processing.
DT=100 µs

0.1

0.2

0.3

0.4
Y(mm)

0.5

0.6

0.7

0.8

0.9

1
0.5 1 1.5 2 2.5
X(mm)
Figure 1 Initial and deformed tagged lines in the continuum regime; Pin 109.6 kPa, Pout 108.5 kPa, T 293 K and
Δt  100 ms. (*), (●) maximum intensity in y direction for the initial and delayed images respectively, ( ) second
order polynomial fit of (●).

In the present paper, a DSMC investigation performed to assist data processing from MTV experiments
is presented. The influence of the degree of rarefaction and of the gas composition is examined. A velocity
reconstruction algorithm, based on the advection-diffusion equation is developed.

2. PROBLEM FORMULATION
The problem encountered in MTV experiments concerns the flow of a binary gas mixture made of background
gas (subscript 1) and tracer (subscript 2) species. The flow is a pressure driven Poiseuille flow. The pressure
difference between the inlet and the outlet of the channel, Pin  Pout, is limited to less than 10 % of the mean
pressure. The inlet, outlet and wall temperatures, Tin , Tout and Tw , are uniform and constant. The flow can be
modeled by two coupled Boltzmann equations [7]:
fi f 2

t r j 1

+ v  i  Qi j ( f j , fi ) , (1)

where v is the velocity, fi (r,v|t) the distribution function of molecular velocity of species i  1; 2  , at the
coordinate r and time t. Molecules are monatomic with a molecular mass mi and a molecular hard sphere
diameter σi. The collision integral Qi j that describes interactions between molecules is given by:
2
1  i   j   f j ( r , w*| t ) f i (r , v*| t ) 
Qi j ( f j , fi )  
2 2  2

3

d 2 kˆ dw 

  f j ( r , w | t ) f i ( r , v | t )
 | vr  kˆ | .


(2)
S R

In Eq. (2) the unit vector k̂ specifies the relative position of two molecules at the time of their collision
with the relative velocity vr = w - v . The post collision velocities v* and w* are defined according to the hard
sphere collision model as [5]:
mj
v*  v  2 (vr  kˆ )kˆ , (3)
mi  m j
mi
w*  w  2 (vr  kˆ )kˆ , (4)
mi  m j

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The macroscopic quantities associated with the mixture flow, i.e. the density ρ, the velocity u and the
temperature T are obtained as the zero, first and second moments of the distribution function, respectively.
Partial and total number and mass densities are respectively defined as:
2
ni ( r, t )   fi ( r , v | t )dv , n ( r , t )   ni ( r , t ) (5)
i 1
2
 i ( r , t )  mi ni ( r , t ) ,  ( r , t )    i ( r , t ) (6)
i 1
Average velocity of each component i is obtained as:
1
ni (r , t ) 
ui  vfi (r , v | t )dv. (7)

The hydrodynamic velocity associated with the overall local mixture momentum is defined as:
2

  (r, t )u (r, t )
i i
uhyd ( r , t )  i 1
(8)
 (r, t )
Single component temperature Ti and overall temperature T can be associated to the velocity dispersion with
respect to the hydrodynamic velocity:
3 1
 
2
ni (r , t )k BTi (r , t )  mi  v  u hyd f i (r , v | t ) dv (9)
2 2
2
3 1

n(r , t )k BT (r , t )   mi  v  u hyd f i ( r , v | t )d v
2
(10)
2 i 1 2

The reflection of the molecules at the wall is modeled as fully diffuse. The distribution function of the reflected
molecules of each species is a Maxwellian fwi at wall temperature Tw defined as:
n (r , t )  v² 
f wi ( rp , v | t )  wi p 3/2 exp    for v  n  0 (11)
(2 RiTw )  2 RiTw 

3. DESCRIPTION OF THE DIFFUSION EFFECT

3.1 Advection-diffusion equation

We consider a steady slow flow in a long rectangular channel, whose length, height and width are Lx, Ly and
Lz, respectively (Figure 2). The pressure difference between the inlet and the outlet of the channel, Pin  Pout,
is considered small. Accordingly the flow can be assumed isothermal, with a small axial density gradient.

Figure 2 Sketch of Poiseuille flow and system coordinate

The velocity field far from the channel ends reduces to its axial component u x ( y , z ) , not dependent on the
axial coordinate x. When the tracer species and tagged molecules concentration are negligibly small then
Eq. (1) shows that tagged molecules transport is governed by the linear Boltzmann equation:
f 2 f
+ v  2  Q21 ( f1 , f 2 ) (12)
t r
Where f1 is the distribution function of the background undisturbed flow, governed by the steady nonlinear
Boltzmann equation for a single species:

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f1
v
 Q21 ( f1 , f1 ) (13)
r
Eqs. (12, 13) describe the diffusion of tracer species through a non-equilibrium background gas. The
reconstruction of the velocity of the background gas through the solution of Eq. (12) is not an easy task,
therefore a simpler, although approximate, method has been followed. It is assumed that the motion of tagged
molecules is governed by the advection-diffusion equation:
p p
 u x ( y, z )  D 2 p   p (14)
t x
In Eq. (14) which replaces Eq. (12), p (x,y,z,t) is the probability density function (PDF) associated with the
luminescent molecules and D is the diffusion coefficient assumed constant since density and temperature
variations are small. The source term  p describes the decay process of the luminescent molecules and 
is the decay constant. This source term can be eliminated by the following rescaling:
p( x, y, z, t )  exp(  t ) p( x, y, z, t ) (15)
The new unknown p( x, y, z, t ) obeys the equation:
 p  p
 u x ( y, z )  D 2 p (16)
t x
Since the luminescent molecules displacement is small compared with the channel length Lx, the x coordinate
domain is considered as unbounded. Accordingly, p is defined in the domain
  ( x, y, z )  R3 ;    x  ,  Ly 2  y  Ly 2,  Lz 2  z  Lz 2 .
Under the assumption that collisions of luminescent molecules with walls do not cause their deexcitation, the
following boundary conditions can be assigned at the walls:
  p
  0 at y   Ly 2
 y
 (17)
 p
 z  0 at z   Lz 2

The initial probability distribution p ( x, z ) is related to the way molecules are excited by the laser beam. In
0
this work, the initially tagged region is a thin circular cylinder parallel to the y-axis:
1
( x , y , z )  C0
p ( x , z )  V (18)
0  0
0 ( x , y , z )  C0

 
with C0  ( x, y, z )  3 : x²  z ²  r0 2 ,  Ly 2  y  Ly 2 , where r0 is the cylinder radius and V0   r02 Ly
its volume.
In the experimental setup, the displacement sx (y,t) of the tagged molecules is recorded at prescribed time tk
(Figure 1) as a function of y, i.e. along the shortest channel side. The displacement sx (y,t) can be deduced from
the probability distribution p( x, y, z, t ) as follows:
1
sx ( y, t ) 

P y ( y, t )
 x p( x, y, z, t ) dx dz (19)

with
 y ( y, t )  p ( x, y, z , t )dxdz .
P  (20)
Finally, an equation involving the displacement profile sx (y,t) and the velocity field ux is obtained by
multiplying Eq. (16) by x, integrating over x and z and taking into account the boundary conditions. It can be
easily shown that sx (y,t) obeys the one-dimensional unsteady and inhomogeneous equation:
sx  ² sx
 ux ( y)  D (21)
t y ²
sx Ly
associated with the initial condition s x ( y , 0)  0 and the boundary condition  0 at y   .
y 2

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3.2 Velocity reconstruction algorithm

Introducing the proper Green function G ( y , y ', t ) , Eq. (21) can be formally solved in the form:
Ly / 2

sx ( y, t )  
 Ly / 2
G ( y, y ', t ) u x ( y ') dy ' (22)

The velocity profile can be obtained from the displacement profile by inverting Eq. (21). However, in practice,
the noise associated with experimental measurements makes the inversion inaccurate. Actually, the diffusion
process makes disturbance decay exponentially in time. The presence of short wavelengths in the displacement
profile as a result of experimental noise makes the inversion amplify them exponentially to such an extent that
the velocity is completely hidden by noise. Although displacement data filtering before inversion could
mitigate the problem, a viable and simple alternative procedure can be devised as follows:
Let Uk (y) for k  0, 1,… , Nu be a sequence of Nu assigned basis functions (typically polynomials). It is assumed
that the gas velocity can be approximated by a linear superposition of these basis functions:
k  Nu
ux ( y)  aU
k 0
k k ( y) (23)

The linearity of the relationship between sx (y,t) and ux (y), expressed by Eq.(21), immediately shows that:
k  Nu Ly /2

sx ( y, t )   a S ( y, t )
k 0
k k with Sk ( y, t )   G ( y, y ', t )U k ( y ')dy ' (24)
 Ly /2

In words, the displacement can be written as a superposition of Nu assigned basis displacements Sk (y,t),
each of them is obtained by solving Eq. (21) with the corresponding velocity Uk(y).The coefficients of the
superposition ak are the same used in Eq. (23), to obtain the velocity, ak can be easily obtained by least square
approximation.

4. NUMERICAL INVESTIGATION
4.1 Numerical method

The system defined by Eq.(1) is solved by DSMC, which is a molecular-based method introduced by Bird [1]
and initially developed for solving hypersonic rarefied flows. In the last decade, DSMC was widely used for
solving MEMS problems [11]. The method numerically solves the dynamic equations (1) where the
distribution function is represented by thousands of simulated molecules, each of them representing a large
number of real molecules. Simulated molecules evolve in time on a sequence of time steps, each time step
consisting of two sub-steps: free flight and local binary collision. The former corresponds to the streaming
operator at the l.h.s of Eq. (1), whereas the latter is performed according to stochastic rules, consistent with the
structure of the collision terms given by Eq. (2). To ensure a successful decoupling of the free flight and the
collision sub-steps, the time step must be smaller than the mean free time (m.f.t.), i.e. the mean time between
two successive collisions of a molecule. The calculation domain is initially uniformly filled with a large
number of simulated molecules. At each time step, all molecules move according to their individual velocities,
then interactions with walls are performed according to Eq. (11), then the molecules are re-indexed: molecules
are removed from their former cell and registered in their new cell. In each cell a number of colliding pairs are
selected according to the no-time-counter method and collisions are then calculated according to Eqs. (3)-(4).
These steps are repeated till statistical convergence. The macroscopic flow properties are finally obtained
statistically by sampling molecular properties in each cell according to Eqs. (5) to (10).
In the present work the flow is studied in Cartesian coordinates as shown in Figure 1. Three sets of
geometries have been considered:
i) a 2D pressure driven Poiseuille flow where Lz >> Ly.
ii) a 1D force driven flow where the force is applied only on the background gas molecules, with Lx
>> Ly and Lz >> Ly.

4.2 DSMC simulation of tracer species diffusion

The role of DSMC simulations in the research activity described here is twofold. The first one is to provide
numerical solutions of the system of Boltzmann equations governing the motion of background and tracer gas,
without assumptions beyond those intrinsic in the kinetic model itself. The second one is to provide well

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controlled simulations of tagged molecules diffusion in order to assess the accuracy of the velocity
reconstruction method described above and to study the influence of the gas rarefaction degree and wall
interaction. It is worth observing that the inevitable statistical noise associated with DSMC simulations is a
quite useful feature of the method because it allows investigate the robustness of the reconstruction against
numerical data presenting noise levels made comparable to experimental ones.
As a first example, the 2D pressure driven flow of pure Argon through a channel of finite length. The
simulated molecules are hard sphere and the mean Knudsen number
Knm   Knin  Knout  2   in  out  2 Ly  0.11 , with Ly 0  100 and Lx 0  1000 , being 0 the mixture
mean free path based on spatially averaged fluid density . Tracer species is created by tagging Argon molecules
themselves in a thin rectangular strip, spanning the whole channel width, at a time when steady flow conditions
have been established.
The comparison between the actual displacement profile, sx (y,t), and an estimated displacement profile
simply obtained from the velocity field, uxhyd t, is shown in Figure 3. Figures 3.a and 3.b respectively show the
displacement profiles captured at t  20 m.f.t. and t  100 m.f.t., normalized by the inlet mean free path in .
sx(y,t)/λin |Ux(hyd)t

y/λ0 y/λ0

Figure 3 Comparison between the actual displacement profile sx (y,t) / λin (●) and the estimated displacement profile uxhyd
t (−), with Kn  0.11 at t  20 m.f.t (a) and at t  100 m.f.t. (b).

A deviation is observed between the actual and estimated displacement profiles. In fact, the actual displacement
profile is affected by the molecular diffusion resulting from the Brownian motion of tracers molecules. The
deviation is more pronounced in the near-wall region where the velocity is low and the diffusion effect is
predominant compared with the advection effect. The former effect increases with the degree of rarefaction of
the gas. The values of the parameter
1
Ly / 2
u xhyd ( y )  sx ( y ) t
Ly  Ly / 2 u xhyd ( Ly / 2)
 dy (25)

that expresses the deviation between actual and estimated profiles is presented in Table 1 as a function of the
mean Knudsen number.

Knm 3.67E-03 5.50E-03 1.10E-02 2.20E-02

ε 0.022 0.026 0.063 0.129
Table 1 Parameter ε as a function of Knm at t  20 m.f.t.

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4.3 Application of the velocity reconstruction algorithm to DSMC data

Two dimensional DSMC simulations, although closer to the real flow geometry, are relatively expensive.
However, a realistic geometry is not strictly necessary to assess the capabilities of the velocity reconstruction
method outlined above. The results presented below are therefore based on simpler one-dimensional
simulations of Poiseuille flows of a binary mixture of hard sphere gases trough the gap between two infinite
parallel walls. The fluid is put into motion by a constant and uniform force field F  Fx xˆ acting on the
background gas.

(a) (b)
Figure 4 Comparison of DSMC (circles) and advection-diffusion equation (solid lines) predictions of tagged molecules
displacements

It is assumed that gas-wall interaction is described by Maxwell model, being Tw and α the walls temperature
and the common value of accommodation coefficient [2] for both species. A reference Knudsen number is
defined as Kn  0 / Ly . Each simulation is split into two phases. During the first one the gas mixture reaches
its steady flow condition. At the beginning of the subsequent phase, the initial position of each tracer molecule
is recorded and used to compute the time evolution of tagged molecules average displacements sx(y,t). During
the second phase, macroscopic properties are also computed by time averaging molecular microscopic
properties. Tagged molecules diffusion and velocity reconstruction by the method described in section (3.2)
have been studied in the following three cases:
1. Tagged species coincides with background gas: m2 / m1  1,  1 /  2  1.
2. Argon-Acetone mixture m2 / m1  1.45 ,  2 /  1  1.88 and  2  0.05.
3. Helium-Acetone mixture: m2 / m1  14.5 ,  2 /  1  3.14 and  2  0.05.
In the last two cases, hard sphere diameters ratios have been estimated from transport properties values at
standard pressure and temperature condition. The tracer species molar concentration  2 has been set equal to
0.05. For each case, the reference Knudsen number has been varied from 0.1 down to 0.01; full accommodation
(α = 1) has been assumed to occur at walls.
DSMC simulations have also been used to determine effective values of the tagged molecules diffusion
coefficient Deff from Einstein's relationship Var ( x)  2 Deff t , relating Deff to the time evolution of the variance
of position variable x during the tagged molecules diffusion through the gas at rest. Although for large Lx the
effective Deff is very close to the value predicted by the Chapman-Enskog expansion for the unconfined fluid
[7], in general its value is affected by the presence of walls [4]. Computed Deff values are reported in Table 2.
Figure 4 shows tagged molecules displacements as predicted by DSMC simulations and by the advection-
diffusion equation in which the proper value of the effective diffusion coefficient Deff has been set. It is also
necessary to take into account that the force field F, although not acting on the tracer species, introduces a
modification of the tracer species velocity which differs from the main velocity field ux(y) by the y-independent
m
amount U F  Deff T FB [7]. The correction UF is only needed when Kn is higher than 0.05. In this case it does
kT
not exceed 1% of the real average flow velocity.

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sx(y,t)/λ0

y/λ0 y/λ0
(a) (b)
Figure 5 Application of velocity reconstruction algorithm to Argon-Acetone mixture. (a)- Reconstructed velocity profiles
from molecules average displacements (solid lines) compared to DSMC velocity profile (filled circles). (b)- Acetone
molecules average displacement profiles at different times from DSMC simulations (circles); solid lines represent best fit
approximations to DSMC data by basis functions Sk.

As shown in Figure 4.b, the advection-diffusion equation provides fairly good predictions of the time evolution
of average molecular displacements for quite different values of mixture mass ratio and Knudsen number. The
application of the algorithm to reconstruct the background gas velocity profile from tagged molecules
displacements is shown in Figure 5 in the case of Argon-Acetone mixture. The Knudsen number is relatively
small, Kn = 0.02. It has been assumed that the velocity profile can be expressed as the sum of just two basis
functions as:
4 y ( Ly  y )
ux ( y )  a0  a2 (25)
L2y
The corresponding displacement basis functions S0(y,t) and S2(y,t) are computed from the advection-diffusion
equation as described above. As shown on Figure 5.a , the velocity profiles reconstructed from DSMC
displacements at different times are almost coincident and in very good agreement with the DSMC computed
velocity profile, in spite of the noisy displacements data used for reconstruction. However, as shown in Figure
6, the reconstruction becomes more problematic at higher Knudsen numbers, where the diffusion effects
dominate advection and displacements profiles become quickly very flat. In these conditions, even a modest
noise level can impair velocity reconstruction. Actually, the velocity profile at 103 mean free times
considerably differs from the reference velocity profile.

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sy(y,t)/λ0

y/λ0 y/λ0
(a) (b)
Figure 6 Application of velocity reconstruction algorithm to Argon-Helium mixture. (a)- Reconstructed velocity profiles
from molecules average displacements (solid lines) compared to DSMC velocity profile (filled circles). (b)- Acetone
molecules average displacement profiles at different times from DSMC simulations (circles); solid lines represent best
fit approximations to DSMC data by basis functions Sk.

Pure Argon a Argon-Acetone c Helium-Acetone c

Kn Deff εv Deff εv Deff εv
0.01 0.95 0.01 0.44 0.01 0.15 0.01
0.02 0.94 0.02 0.43 0.008 0.146 0.005
0.04 0.93 0.034 0.425 0.03 0.145 0.012
0.05 0.93 0.08 (0.03)b 0.422 0.04 0.144 0.035
0.1 0.903 0.37 (0.18)b 0.42 0.18 0.142 0.03
Table 2 Effective diffusion coefficient Deff and velocity reconstruction error εv as a function of the Knudsen number for
three mixtures. a 800 particles/cell, b 8000 particles/cell, c 2×106 mixture overall simulation particles number. Deff valued
normalized by setting 0  1, m1  1 and k BTw  1 , kB is the Boltzmann constant.

It is useful to define the error associated with the reconstruction algorithm as:
1
Ly /2
u x( r ) ( y )  u x ( y )
Ly  Ly /2 u x ( Ly / 2)
v  dy (25)

Where ux( r ) ( y) and ux(y) are the reconstructed and reference velocity profiles respectively. Table 2 shows the
effects of Knudsen number and mixture properties on the reconstruction error. Increasing Kn makes
reconstruction more difficult for the reason mentioned above when commenting Figure 6. As shown by the
errors obtained by using 800 and 8000 simulation particles per cell, decreasing the statistical noise allows
smaller εv (as is obvious) but the mixture diffusion coefficient plays also an important role, since smaller tracer
particles diffusion has an obvious beneficial effect on velocity profiles reconstruction.

5. CONCLUSIONS
DSMC results show that the displacement profile is affected by the molecular diffusion, the diffusion effect
cannot be ignored at moderate and high Knudsen numbers in molecular tagging velocimetry analysis. A simple

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algorithm based on the advection-diffusion equation has been developed to obtain the velocity profile from the
displacement field of the tagged molecules.
The application of the reconstruction algorithm to displacements obtained numerically by DSMC shows
that the reconstruction becomes more difficult as the Knudsen number increases. It should be noted that, when
the degree of gas rarefaction increases, the diffusion equation approximation requires the adoption of an
effective diffusion coefficient which also takes into account the presence of the diffusion Knudsen layers [4].
As expected, the reconstruction error gets smaller when the binary background-tracer diffusion coefficient is
reduced.
Although the reconstruction algorithm is validated with DSMC data, a further validation with MTV
measurements is required.

ACKNOWLEDGEMENTS
This research obtained financial support from the European Community's Seventh Framework Program
(FP7/2007-2013) under grant agreement no 215504, from the Fédération de Recherche Fermat, FR 3089, and
from the Project 30176ZE of the PHC GALILEE 2014 Program. The latter is supported by the Ministère des
Affaires Etrangères et du Développement International (MAEDI) and the Ministère de l’Enseignement
Supérieur et de la Recherche (MENESR).

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