SCIENCE CHINA

Technological Sciences
• RESEARCH PAPER • July 2013 Vol.56 No.7: 1607–1617
doi: 10.1007/s11431-013-5237-y

Simulations of mixing processes after coalescence of binary

momentum-less droplets
LIU Dong, GUO YinCheng* & LIN WenYi
School of Aerospace, Tsinghua University, Beijing 100084, China

Received January 7, 2013; accepted April 16, 2013; published online May 24, 2013

The fate of the internal fluids after coalescence of droplets is very important and has been investigated rarely. In this paper, we
report simulations of mixing processes after coalescence of binary momentum-less droplets by using a front tracking method.
Firstly, the validation of the method used here was testified, and then the effects of viscosity of droplets, size ratio and proper-
ties of ambient phase on mixing were investigated. The results qualitatively agree well with previous experimental observa-
tions.

droplet coalescence, mixing, front tracking

Citation: Liu D, Guo Y C, Lin W Y. Simulations of mixing processes after coalescence of binary momentum-less droplets. Sci China Tech Sci, 2013, 56:
16071617, doi: 10.1007/s11431-013-5237-y

1 Introduction binary droplets or droplet with liquid interface [5–12],

however these researches mainly focus on the outcomes of
collision (bounce, coalescence or partial coalescence). As
Droplet coalescence is a common phenomenon and essen-
this is a multi-scale complex problem, so far there is no
tial feature in many industrial processes such as various
perfect explanation and model that can precisely predict the
applications of interest to chemical engineers including liq-
outcomes. Anilkumar et al. [13] firstly studied the coales-
uid-liquid extraction, emulsification, spray coating, hydro-
cence and the subsequent internal fluids flow of initially
carbon fermentation and waste treatment [1, 2]. Earlier
stationary binary droplets of unequal sizes by experiments.
studies on this topic have focused on the evolution of the
They reported a high-speed video sequence showing the
drop interface, which is the easiest aspect to observe ex-
coalescence of two different-sized drops (4.85 and 2.33 mm)
perimentally. However, the fate of the internal fluids after
of low viscosity. It was found that there was considerable
coalescence and how well they become mixed are of greater
mixing following coalescence. The smaller drop penetrated
practical importance, such as the success of liquid-liquid
the larger drop in the form of a vortex. The coalesced drop
extraction operations depends on the rate of mass transfer
also underwent shape oscillations. Whereas, at higher drop-
after droplets coalescence [3], extensive and rapid mixing
let viscosity, there was no noticeable penetration. The
after coalescence so as to facilitate reaction desired for high
smaller drop fluid formed a blob which was simply lodged
viscous gelled hypergolic propellants (GHPs) and ionic liq-
in the larger drop. Nobari and Tryggvason [14] numerically
uids (ILs) [4].
repeated these same results by using a front tracking method.
Many researches have been carried out on coalescence of
For low Ohnesorge number, their simulation results show
that the small drop forms a jet that penetrates far into the
large drop. This jet can lead to a relatively large mixing
*Corresponding author (email: guoyc@tsinghua.edu.cn)

© Science China Press and Springer-Verlag Berlin Heidelberg 2013 tech.scichina.com www.springerlink.com
1608 Liu D, et al. Sci China Tech Sci July (2013) Vol.56 No.7

between the fluids from the small and the large drops. For 1  
high Ohnesorge number, little mixing takes place and the rvr  vz  0. (2)
r r z
small drop fluid forms a blob near the point where the drops
touched initially. Blanchette [15] numerically simulated Furthermore, the density and viscosity are assumed to be
initial stationary coalescence of binary droplets with differ- constants in each phase.
ent size and surface tension coefficient. Compared with the A fixed staggered grid is used to compute the velocity
effect of different surface tension coefficient, size discrep- and pressure field. The equations are solved by a projection
ancies were not found to generate significant mixing. Ref. method: at each time step, we first find a temporary velocity
[4] reported the development of the mixing process subse- field u* by ignoring the pressure term, and then we find the
quent to coalescence for binary droplets of unequal sizes. actual velocity by adding the pressure term:
They found that jet emerged, disappeared and emerged
t
again as the impact inertia increased. In order to keep the u(t  t )  u*   h P, (3)
total energy conserved for droplet coalescence with initial  n 1
velocity, Liu et al. [16] developed a numerical method in where P is solved via a pressure Poisson eq. (4) by a simple
which they transferred the energy of merged surface to ki- successive-over-relaxation (SOR) method.
netic energy of neighboring fluid, and then they found that
this part of energy was critical for the mushroom-like jet 1 1
h h P   h u* . (4)
formation.  n 1 t
In this paper, a front tracking method is used to simulate
the coalescence of binary equal- and unequal-size momen- In the front tracking method, the front is explicitly repre-
tum-less droplets. We pay our attention to the internal fluid sented by discrete points and elements (as shown in Figure
flow pattern and the mixing processes. The reason why co- 1) while this makes the surface tension computations much
alescence of momentum-less droplets was chosen here is to more straightforward than reconstructing it from a marker
avoid the questions about coalescence (whether, when and function.
where coalescence happens). The effects of size ratio, vis- The force on a short element is given by
cosity of droplets, properties of outer fluid phases on mixing
are investigated in detail.
 F    knds. (5)
s

Using the definition of the curvature of a two-dimensional

2 Formulation and numerical specifications s
line, kn  , we can write eq. (5) as
s
The front tracking method adopted herein has been dis-
s
cussed in details by Unverdi [17] and Unverdi and Trygg-  F    knds    ds    s2  s1  . (6)
vason [18]. The computation code we used is an axisym- s s s
metric version of this method. Briefly, both fluids obey the Therefore, the accuracy and efficiency of the surface ten-
Navier-Stokes equations and are solved by one set of equa- sion computations depend on how we find the tangent vec-
tions: tors. In ref. [18], the tangents of the front were calculated

 vr 1  
 r  vr2   vz vr
t r r z
p  v  v 
   2 r  2  r 
r r r r  r 
  vz vr 
    Fr , (1)
z  r z 
 vz 1  
 r  vz vr   vz2
t r r z
p 1   vz vr   v
  r   2  z  Fz ,
z r r  r z  z z

where Fr, Fz is the surface tension force and only acts where
the fluid interface is, and the gravity is ignored here. Both
the fluids are assumed to be incompressible, so the continu- Figure 1 Computations of flow containing two phases and the structure
ity equation gives: of front.
 Liu D, et al.
directly from cubic polynomial fitting through four end
points of the element and the adjacent element of the front.
In this paper, the least-square polynomial fitting was used
by six points in order to increase the simulation accuracy
and stability.
Since the extent of mixing of the fluids is the key issue in
the present study, an illustration of the mixing process is
conducted by tracing mass-less particles in a Lagrangian
frame, even though binary droplets are composed of the
same liquid. Specifically, at every time step the velocity of a
tracing particle (totally 5000 particles used in the simul-
ation) is calculated by interpolating from the neighboring
Eulerian velocities node. Then the particle is moved to its
new location using the following explicit scheme:
ri (t  t )  ri (t )  vi t ,
where ri and vi denote the position and velocity of the parti-
cle i, respectively.
3 Results and discussion
The main parameters describing the coalescence of binary
initially stationary droplets are: the large and small droplets
diameters (dl, ds), the density, viscosity and surface tension
coefficient of droplets (d, d, ) and the density and vis-
cosity of outer fluid (o, o). Hence d c  (d l3  ds3 )1/3 is the
diameter of the coalesced droplet. The non-dimensional
parameters controlling the droplet coalescence are the size
d d
ratio   s and the Ohnesorge number Oh  ,
dl  d d c
which relates the viscous forces to inertial and surface ten-
sion forces. After the droplets coalesce, the combined drop-
π d dc3
let oscillates.   , which corresponds to the
4 
lowest mode of natural oscillation of the merged droplet, is
used in our investigation as time unit.
Figure 2 shows a sketch of the computational setup. In all
of our simulations, we fix the diameter of the merged drop-
let as d c  (23  23 )1/3 and put the merged droplet in the
center of the simulation domain in order to decrease the
boundary effect. The domain size is fixed at 4×8 in all our
simulation cases.
Initial coalescence of binary droplets is modeled by
opening a small hole and the binary droplets are connected
as one droplet. The fluids inside and outside droplets are
assumed to be at rest as illustrated in Figure 2. We exam-
ined the effect of the size of this opening and found that
once it was sufficiently small, as it was here, the resulting
motion was independent of its size.
Sci China Tech Sci July (2013) Vol.56 No.7 1609
Figure 2 Sketch of the computation setup.
(7)
3.1 Validation
Firstly, the liquid-liquid system is considered. In other word,
the density and viscosity of fluid inner and outer droplet are
taken as the same if without special instruction. The coales-
cence of binary equal-size droplets with Oh=0.01 is simu-
lated.
We begin by verifying the conservation of mass (vol-
ume) of the merged droplet and energy at various resolu-
tions, 100×200, 200×400, 266×532, corresponding to
r=z=0.04, 0.02, 0.015. The droplet volume is well con-
served even at fairly low resolutions, with maximum error
within 0.03% as shown in Figure 3(a). The total energy of
the flow field consists of surface energy, kinetic energy, and
the cumulative viscous dissipation energy. In all our simula-
tions, we did not solve the energy conservation equation. So
kinetic energy and cumulative viscous dissipation energy
were evaluated through the velocity field, while surface
energy was evaluated through the surface geometry as in ref.
[19]. The good conservation of total energy with maximum
error within 0.4% as shown in Figure 3(b) in some extent
proved the validity of our simulation. As a result of this
mesh refinement study, r=z=0.02 are selected for all oth-
er calculations in this paper.
Figure 4 shows the evolution of the various energy com-
ponents. Initially, the excess surface energy drops down
very quickly and is transferred to kinetic energy and dissi-
pated energy. Then the droplet oscillates as one droplet with
damping amplitude. Figure 5 shows the evolution of the
droplet surface shape. Initially the droplet merged at nearly
one single point, and then the neck pulled outward very
quickly due to the highly curved meniscus connecting the
two droplets. This very early phase qualitatively agrees with
Menchaca-Rocha et al.’s results as shown in Figure 3 of ref.
[20]. They put mercury droplets on specially treated glass
surface and used fast, digital, and analog imaging tech-
niques to record the images.
Figure 6 depicts the velocity vector field within and
around the droplet. As there is no external force, the veloci-
1610 Liu D, et al. Sci China Tech Sci July (2013) Vol.56 No.7

ty field is perfectly symmetric. As the deformation of drop-
let is caused by the surface tension, the velocity field con-
centrates around the droplet all the time. This implies that
the fluctuation of kinetic energy is mainly caused by the
oscillation of the merged droplet.
3.2 Effect of Oh
In order to investigate the effect of Oh, we simulate a series
of Oh from 0.001 to 0.02 at a fixed medium size ratio 0.5.
Figure 7 shows the evoluation of the merged droplet surface
and internal flow pattern for the case with Oh=0.001. We
can find that a small jet formation from the smaller droplet
goes down very quickly with vortex ring at its tip. At about
t=0.8−0.9, the jet touches the interface of the merged
droplet, then the vortex adjoins the interface and rotates
outward. The fluid from the small droplet forms a channel
while the droplet oscillates and touches the interface at
about t=2.0 again, then rolls up, forming a big vortex with
the small vortex at the end. This process can also be
presented by the velocity vector map and pressure contour
as shown in Figures 8 and 9, respectively. According to
Young-Laplace equation, the smaller droplet has a greater
internal pressure than the larger one. The difference be-
tween pressures is also thought to be a reason for the for-
mation of mixing. It is clear that the zone with high velocity
field always accompanied with big pressures changes as
shown in Figure 9. From this case we can image the high
mixing rate and rapid reaction rate for different kinds of
droplet fluid if the viscosity is small. Figure 10 shows the
case with Oh =0.02. We can find that the evolution of the
interface and the internal flow are distinctly different with
Oh=0.001. The deformation of the interface is not as violent
as the small Oh case that is because of the high viscosity of
the ambient phase. There is no jet formation and the fluid
from the smaller droplet just forms a blob and lodges in the
larger droplet.
Figure 11 shows the eventual situation (almost) of
different Oh. It is very clear that as the Oh decreases, the
penetration length and mixing efficiency increase. Figure 12
shows the evolution of kinetic energy and viscosity dissip-
ation rate with different Oh. It is very easy to understand
that the kinetic energy decreases slowly while Oh is low.
The multimodal characteristic of kinetic energy disappears
later if Oh is low and if there is vortex. Initially, the visco-
sity dissipation rate is high if Oh is high and then decreases
at later stage. That is because of the balance between
velocity and viscosity, initially the velocity on the same
scale, and then the velocity decreases quickly if the viscos-
ity is high.

Figure 3 Time evolution of (a) the merged droplet volume and (b) the total energy calculated at different resolutions.

Figure 4 Energy budget of coalescence of binary stationary equal-size droplets with Oh=0.01. KE denotes the total kinetic energy; DE, the total dissipation
energy; SE, the surface energy; TE, the total energy, and VDR is the viscous dissipation rate, each normalized by the initial energy.
 Liu D, et al. Sci China Tech Sci July (2013) Vol.56 No.7 1611

Figure 5 Time sequence for the coalescence of binary droplets with =1.0, Oh=0.01.

Figure 6 Time sequence of velocity vector field.

1612 Liu D, et al. Sci China Tech Sci July (2013) Vol.56 No.7

Figure 7 Time sequence for the coalescence of binary droplets with =0.5, Oh=0.001.

Figure 8 Time sequence of velocity vector field.

 Liu D, et al. Sci China Tech Sci July (2013) Vol.56 No.7 1613

Figure 9 Time sequence of pressure contour.

Figure 10 Time sequence for the coalescence of binary droplets with =0.5, Oh=0.02.

Figure 11 Internal flow at t=6.0 for different Oh with size ratio =0.5.

Figure 12 Time evoluation of kinetic energy and viscous dissipation rate.

1614 Liu D, et al. Sci China Tech Sci
3.3 Effect of size ratio
The final states (almost) of bianry droplets coalescence with
different size ratios (=0.8, 0.7, 0.2, 0.3, 0.2) are shown in
Figure 13. We choose two Oh numbers here, 0.005 and 0.01.
It is obvious that the increase of size discrepancy can
increase mixing firstly then the effect decreases because if
the small droplet size is too small it cannot cause large
impact to the large droplet. We must notice that the mass
ratio is of three-square of size ratio, for the size ratio 0.2,
the small droplet is just 0.8% of the large one. The
definition of Oh here is different from that defined in refs.
[14, 15], we used diameter of the merged droplet, while ref.
[14] used diameter of small droplet and ref. [15] used radius
of small or large droplet. Oh must be magnified with diff-
erent ratios in order to compare with their results. So it is
not rational as reported in ref. [15] size discrepancies were
not found to generate significant mixing with the parameter
scales they used. That may be because of the high dissipa-
tion characteristic of their numerical method.
For different size ratios, the initial surface energy (total
energy) is not the same, so in this part we use the surface
energy of the merged droplet at equilibrium state as energy
unit. From the surface energy as shown in Figure 14, we can
find that the surface energy drops down very quickly at a
Figure 13 Internal flows at t=6.0 for different size ratio.
Figure 14 Time evolutions of surface energy for differnt size ratio .
July (2013) Vol.56 No.7
approximately same speed. Then for larger size ratio, the
oscillations of the merged droplet are both larger in amp-
litude and with longer damping time. Figures 15 and 16
show the evolutions of kinetic energy and viscous dissipa-
tion rate, respectively. From the kinetic energy, we can find
that the oscillation period of the merged droplet is nearly
equal for different size ratios, however the multimodal
characteristic exists for the little size ratio, which may be an
indicator as we metioned in Section 3.2.
3.4 Effect of ambient phase properties
The coalescence of liuqid droplets most happens in liquid
phase for the application of some chemisty processes, liq-
uid-liquid extraction, emulsification and so on. However for
the application of combustion engine, gelled hypergolic
propellants and spray coating etc., the coalescence of liquid
droplets happens in gas phase. Therefore, in this section, we
investigate the effect of ambient phase properties. We mod-
el gas phase by taking both the density and viscosity of am-
bient phase as 1% of the liquid droplet phase. Figures 17
and 18 show the time sequences for coalescence of binary
droplets with size ratio 0.5 in liquid/gas phase with two
kinds of Oh, 0.01 and 0.005. Compared with gas phase, we
can find that the high density and viscosity of liquid phase
 Liu D, et al. Sci China Tech Sci July (2013) Vol.56 No.7 1615

Figure 15 Time evolutions of kinetic energy with differnt size ratios .

Figure 16 Time evolutions of viscous dissipation rate with differnt size ratios .

Figure 17 Time sequence for the coalescence of binary droplets with =0.5, Oh=0.01.
1616 Liu D, et al. Sci China Tech Sci
Figure 18 Time sequence for the coalescence of binary droplets with =0.5, Oh=0.005.
lead to a high damping of the droplet oscillation, but have
little effect on the mixing process. The deformation of
droplet in gas phase is a little more violent than in liquid
phase, which is more obvious in the early phase as shown at
the time of 0.1 and 0.2 of Figures 17 and 18, respectively.
The stretch of little droplet is longer in gas phase compared
with that in liquid phase for both Oh=0.01 and 0.005. There
is a little difference for the mixing process which means
oscill- ation cannot facilitate mixing.
Figures 19 and 20 show the evolutions of kinetic energy
and surface energy for the cases simulated in Figures 17 and
18, respectively. From the kinetic energy, the effect of am-
bient phase properties on oscillation is clear. The oscillation
period and damping velocity of droplet in gas phase are
smaller than those in liquid phase. That is very easy to
understand because the density and viscosity of gas are both
smaller than those of liquid. From the surfcae energy, we
can find that the initial decrease of surface energy for
droplet in liquid phase is just a little faster than that in gas
phase. It implies that the initial deformation of the merged
droplet is dominated by the surface tension force so the
July (2013) Vol.56 No.7
deformation processes of the merged droplets are similar.
This also explains why the initial deformation processes as
we show in Figure 5 are similar to Menchaca-Rocha et al.’s
[20] results.
4 Concluding remarks
The front tracking method has been applied to the simul-
ation of coalescence and mixing of binary droplets with
different size ratio. The effect of Oh, size ratio, and the
properties of ambient phase have been revealed in detail.
The computations show that for low Oh or viscosity of
droplets with intermediate size ratio, the fluid from the
small droplet forms a jet and penetrates far into the large
one and rolls up, which undoubtedly can lead to large
mixing between the fluids from the small and large droplets.
However, for large Oh or viscosity of droplets, the fluid
from the small droplet cannot penetrate the large one and
just forms a blob and simply lodges in the large one. These
results are in accordance with previous experiments [13]
 Liu D, et al. Sci China Tech Sci
Figure 19 Time evolutions of kinetic energy and surface energy with =0.5, Oh=0.01.
Figure 20 Time evolutions of kinetic energy and surface energy with =0.5, Oh=0.005.
and numerical results [14]. Besides, we have examined the
effect of size ratio and have found that increase of size
discrepancies can increase mixing firstly then decrease the
effect.
At last, we have examined the effect of ambient phase
and simply classified ambient phase to liquid and gas. The
results show that the ambient phase plays a fundamental
role in the droplets oscillation but has no help to facilitating
mixing. These results have great enlightment to various
engineering applications.
The results provide a description of coalescence and
mixing of binary droplets in detail. But because we have not
found a proper parameter to measure the mixing, we can
just investigate the effect of various properties on mixing
qualitatively. Quantitative analysis needs a lot of work in
future.
This work was supported by the National Natural Science Foundation of
China (Grant No. 51176099). We thank Prof. C. K. Law and Dr. Zhang
Peng for helpful discussions.
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