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Magnetic Instruments _______________________________________________________

Control of Ferrofluid Droplets in Microchannels by Uniform Magnetic Fields

Vijaykumar B. Varma1, Ayan Ray1, Zhaomeng Wang1, Zhiping Wang2, Ruige Wu2, P. J. Jayaneel3,
Natteri M. Sudharsan3, and Raju V. Ramanujan1*
1
School of Materials Science and Engineering, Nanyang Technological University, Singapore, 639798
2
Singapore Institute of Manufacturing Technology, 71 Nanyang Dr, Singapore 638075
3
Department of Mechanical Engineering, Rajalakshmi Engineering College, Chennai, India, 602105
*Member, IEEE

Abstract— Magnetic droplets are versatile tools for a range of Lab-on-a-chip (LoC) applications. The combination of a
uniform magnetic field and magnetic droplet offers wireless and programmable manipulation. We performed LoC
experiments and numerical studies on ferrofluid droplets under the influence of a uniform magnetic field. The dynamic
behavior of flowing ferrofluid droplets was examined. The droplet size, shape, inter droplet spacing and velocity could
be controlled by tuning the magnetic susceptibility of the ferrofluid, the viscosity of the carrier medium, and the flow rates.
Our droplet-based micro-magnetofluidic numerical model is in good agreement with our experiments. These studies are
useful for magnetic droplet control and mixing in a LoC using a uniform magnetic field.

Index Terms— Magnetic instruments, droplet micro-magnetofluidics, ferrofluid droplets, LoC manipulation, uniform magnetic fields.

I. INTRODUCTION droplet manipulation by the magnetic field from a permanent magnet

Droplet-based microfluidics [1, 2] offers a versatile technique for
carrying out multiple reactions in several, small, isolated, containers.
Miniaturization due to microfluidics provides the capability for
multiplexing; several parallel processes can be implemented on a Lab-
on-a-Chip (LoC) platform. One can use these platforms to carry out
sensing [3, 4], fabrication of microparticles [5-7], bacteria trapping
[8] and combinatorial chemistry for drug discovery [9]. The droplet
microfluidics approach on a LoC platform provides a flexible
fabrication technique for controlled particle fabrication [6] e.g.,
fabrication of Janus structures [7], anisotropic particles [10],
polymeric structures [11], controlled encapsulation for drug delivery
[12] and multidimensional optical barcoding [13].
These capabilities can be enhanced by controlling the droplet
movement and shape. Wireless control and remote manipulation of
the ferrofluid droplets by an applied magnetic field provides such a
capability. A few studies have been reported on ferrofluid droplet
(dispersed phase, DP) manipulation when the continuous phase (CP,
oil) has motion relative to the ferrofluid droplets (dynamic continuous
phase, dCP). Droplet breakup [14], ordered arrangement of the
droplets[15], droplet dynamics in a magnetic field gradient[16, 17]
and various numerical modelling investigations [18-20] have been
reported. Wu et al. reported the use of both uniform and non-uniform
magnetic fields generated by a combination of two permanent
magnets to demonstrate active control of the breakup of the ferrofluid
droplets in a T-junction [14]. They concluded that the uniform
magnetic field can influence the stretching and breakup process of the
droplets. Non-uniform magnetic fields can result in asymmetrical
breakup, resulting in droplets of different sizes. Lee et al. reported the
generation and distribution of droplets under an external magnetic
fields in a microfluidic T-junction [21]. The kinematic behavior of
ferrofluid droplets under magnetic fields from planar coils [16],
[17] and formation of droplets due to uniform magnetic fields [19]
have been reported. Ferrofluid droplet formation in the presence of
pressure drop, viscous drag, and interfacial tension have been studied.
Increasing the interfacial tension reduces the droplet deformation;
increasing the pressure drop and viscous drag increases the force on
the droplet. An external magnetic field which is in the direction of the
viscous drag adds to the volume force acting against interfacial
tension, resulting in larger droplet volume for higher magnetic Bond
number (ratio of magnetic force and surface tension force) and higher
susceptibility of the ferrofluid [19]. Ferrofluid droplet behavior on a
LoC platform in the presence of a uniform magnetic field has not been
adequately explored (for the dCP case). Further, manipulation of
ferrofluid droplets by a uniform magnetic field has not been
demonstrated on a LoC platform.
Our studies report the effect of a uniform magnetic field on the
motion, size and shape of ferrofluid droplets generated by a T-
junction in a LoC platform. Our numerical and experimental studies
demonstrate the effect of viscosity (η), flow rate ratio (Qr) and
magnetic susceptibility of the ferrofluid (χ) on droplet behavior in the
presence of the applied uniform magnetic field (ℋ). The flow rate
ratio is defined as the ratio of the flow rate of the CP (Qcp) to flow rate
of the DP (Qdp). These studies are useful for wirelessly controlled
manipulation of the droplets and magnetically controlled Janus [7]
particle formation, which can be used for magnetically controlled
reaction kinetics, biosensing and drug delivery applications.
II. EXPERIMENTAL
The effect of a uniform magnetic field on the ferrofluid droplets
was studied using: (i) a microfluidic chip, (ii) materials for droplet
generation and (iii) a micro-magnetofluidic setup [22, 23]. The
droplets were generated by a T-junction configuration with

Corresponding author: R. V. Ramanujan (ramanujan@ntu.edu.sg)

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immiscible phases of the CP and the DP (Fig. 1a). A magnetic field
ℋ was applied perpendicular to the droplet flow and high-speed
imaging was performed. Droplet shape deformation, motion and size
were quantified by measuring the aspect ratio of the droplets (ARD),
inter droplet spacing (IDS), velocity (VOD) and the perimeter of the
droplets (POD), respectively.
Fig. 1. (a) Schematic of droplet generation (not to scale). (b) Outline
of micromagnetofluidic setup. (c) Geometry of experiment and
numerical model, with simulation results for S1Qr50. Scale in mm,
scale bar=500μm. (d) Experimental micrographs of ferrofluid
droplets in uniform magnetic field for set S1Qr10 and S1Qr50. (e-f)
Comparison of experimental (e) and simulated (f) droplet deformation
in magnetic fields. For experiments (c, d, e), DP is in black color and
CP is transparent. For simulations (c, f), blue denotes DP and red
denotes CP.
A. Microfluidic Chip
Droplets were generated by a 250 μm×250 μm T-junction, in a
thermally bonded (Specac, Atlas 15T) poly(methyl methacrylate)
microfluidic chip [24]. AutoCAD 2015 was used for the
75mm×25mm chip design and fabricated by a micro-milling
technique. It consists of two inlets (for DP and CP) and one outlet, all
with 250 μm depths and 500 μm widths.
B. Materials
The droplets were generated using two immiscible phases:
ferrofluid (DP) and oil (CP) (Fig. 1a). The effect of viscosity on the
droplet behavior was studied by using two CP’s: 3 mPa.s n-
hexadecane (99%, Alfa Aesar, VWR Singapore) and 18 mPa.s light
mineral oil (Sigma-Aldrich, Singapore). Droplet coalescence was
prevented by adding 1 % SPAN 80 (Sigma-Aldrich, Singapore) to the
CP. The effect of magnetic susceptibility was studied by using two
water-based ferrofluids EMG 607 and EMG 807 (Ferrotec,
IEEE MAGNETICS LETTERS
Singapore) (Table 1).
Table 1. Properties of Water Based Ferrofluids
Quantity EMG 607 EMG 807
Saturation Magnetization (mT) 11 11
Density at 25 oC (kg/m3) 1.1 x 103 1.1 x 103
Magnetic Susceptibility (SI units) 1.63 1.88
Magnetic Particle vol Concentration 2% 2%
Particle Diameter (nm) 10 10
Viscosity (mPa·s) 2 1.8
C. Experimental Setup
The effect of a magnetic field ℋ on the droplets was studied by
using a micromagnetofluidic setup (Fig. 1b), consisting of (i) droplet
generator, (ii) uniform magnetic field, and (iii) high-speed imaging
with image processing. The CP and the DP were injected into the
microfluidic channel by a KDS Gemini 88 syringe pump using two
independent Exmire gastight syringes (1 ml Luer lock), connected by
IDEX tubing (0.50 mm inner diameter, 1.59 mm outer diameter).
A DEXING Electromagnet System (model: DXSB-178) was used
to generate the uniform magnetic field (uniformity of ±0.1 % for a
region 5 mm wide×10 mm long) with an air gap of 4 cm (between
pole pieces). The microfluidic chip was placed in the middle of the
pole pieces. The direction of the magnetic field was perpendicular to
the flow of droplets. High-speed imaging (50 fps, resolution
640×1200 pixels) was performed with a Phantom Miro Camera
(Model: M320s) coupled to a magnifying lens (Navitar Zoom 6000).
The videos were analyzed using ImageJ and Phantom Camera Control
(PCC) software. The ARD, POD and IDS were determined using
ImageJ software. The PCC software was used to measure 10
consecutive VOD. The data points in all of the graphs represent the
averaged values of the measurements and the error bars indicate the
standard error of the mean [25] for the corresponding data points.
D. Experiment Parameters
The experiments were performed with magnetic field ℋ=0, 10, 25,
50, 100, 250, 500 mT. Sets performed at flow rate ratio 10 and flow
rate ratio 50 are indicated by Q1 and Q2, respectively. The viscosity
of hexadecane and mineral oil are indicated by η1 (3mPa.s) and η2
(18mPa.s), respectively. The susceptibility of ferrofluid EMG 607 and
EMG 807 are denoted by χ1 (1.63) and χ2 (1.86), respectively.
Parameters i.e. viscosity, susceptibility, Qr (in the parentheses) of the
performed sets are: S1Qr10 (η1χ1Q1), S2Qr10 (η1χ2Q1), S3Qr10
(η2χ1Q1), S1Qr50 (η1χ1Q2), S2Qr50 (η1χ2Q2) and S3Qr50 (η2χ1Q2).
III. NUMERICAL MODEL
The response of the droplets to an applied magnetic field depends
on the strength and type (uniform or gradient) of the magnetic field.
Rosensweig [26] used a continuum model to explain the phenomena
observed for ferrofluids. Numerical simulations for droplet behavior
in a magnetic field ℋ were performed and compared with the
experimental results (Fig. 1c-1f).
A. Simulation Methodology
A two dimensional (2D) droplet micromagnetofluidic numerical
model (Fig. 1a, 1c) was developed to perform ferrofluid droplet
simulations for the dCP (the CP is in motion) in COMSOL
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Multiphysics software. The experimentally measured values for the
susceptibility, viscosities, densities, flow rates and magnetic fields
were used (Section II-D). The experimental values of the droplet
diameters and droplet spacings were defined in the microchannel and
used as the initial condition (Fig. 1c). An extra-fine mesh (total
elements 30778) was created by triangular elements from 0.25 μm
(minimum) to 21.7 μm (maximum) for the microchannel containing
droplets (19582 elements) and from 1.1 μm (minimum) to 100 μm
(maximum) for magnetic fields (11196 elements). The uniform
magnetic field was simulated by the no-currents method in AC/DC
module along the Y-direction, perpendicular to the X-direction CP
flow (Fig. 1a, 1c). A fully developed CP flow profiles was simulated
by using laminar two-phase flow, level-set method in the fluid
dynamics module, with no slip, laminar inflow boundary conditions.
The simulated movies were exported and analyzed to obtain the
values of the ARD and the VOD.
B. Governing Equations:
1. Equation of motion
η2=18 mPa.s) (Section II-D). Ferrofluids with different
susceptibilities (χ2=1.86, χ1=1.63) were used to study the role of the
magnetic properties (Table 1). Initially, spherical droplets are
generated at the T-junction due to surface tension. When a magnetic
field ℋ is applied, the magnetic body force (equation (4)) acts against
the surface tension force, resulting in elongation of droplets along the
field direction (Fig. 1c-1f).
Figure 2a shows the influence of a magnetic field ℋ on the POD.
The POD increases (set S2Qr10, η1χ2Q1) at low flow rate ratio Qr10.
For a high susceptibility ferrofluid, the magnetic body force at the T-
junction increases by increasing the magnetic field. At Qr10, there is
less drag force from the flow of the CP. Consequently, at the T-
junction, the effect of the magnetic body force is high, leading to
droplet breakup at the larger POD, which increases with increasing
magnetic field. For set S2 at Qr10, a decrease in the POD was
observed by increasing magnetic field from 0 to 50 mT. The POD
increases by increasing magnetic field from 50 to 250 mT and nearly
stabilizes beyond 250 mT.
1300
(a) 1 2Q1 1.6
(b) 1 2Q1

Perimeter of Droplets (m)

Aspect Ratio of Droplets

1200
The equation of motion for ferrofluid droplets is given by [19, 27, 28] , 1 1Q1

𝜌 𝜕𝒖/𝜕𝑡 + 𝜌(𝒖 ∙ 𝜵)𝒖 = −𝜵 𝑝 + 𝜵 ⋅ [𝜂(𝜵𝒖 + (𝜵𝒖)𝑻 )] −

1100
1.4
21Q1
1000
𝜎𝜅𝛿𝑠 𝜵𝜙 + 𝓕𝒎 and 𝜵 ∙ 𝒖 = 0 (1) 900
1 2Q2

1 1Q2 1 2Q2
Where, ℱm is the magnetic volume force, u is velocity, p is pressure, 800
1.2
1 1Q1
1 1Q2
σ is surface tension, κ is curvature and δs is the smoothed delta 700 21Q1
21Q2
function which is zero everywhere except at the interface and ϕ is the 600
2 1Q1
1.0
0 100 200 300 400 500 600
level set function. The density ρ and the viscosity η can be defined by 0 100 200 300
Magnetic Field (mT)
400 500
Magnetic Field (mT)
weighted average interpolation, for a ferrofluid volume fraction ϵ (ϵ=1

Velocity of Droplets (mm/s)

5000 (c) set S1-Qr10
Inter Droplet Spacing (m)

1.4 21Q2 set S1-Qr50

represents DP) [22, 23, 27]: ρ = ρcp(1- ϵ)+ ρdpϵ and η = ηcp(1- ϵ)+ 1 2Q2 set S2-Qr10
4000 1.2
1 1Q2
(d) set S2-Qr50
ηdpϵ. The subscript cp and dp indicate values for CP and DP. 1.0 set S3-Qr10
3000 set S3-Qr50
1 1Q2 0.8
2. Magnetic Force 1 2Q1
1 2Q1
2000 21Q2 0.6
The magnetic field, from Maxwell’s equation for magnetostatics is 0.4
1000 21Q1 21Q1 1 2Q2
given by [26] 1 1Q1
0.2
1 1Q1
∇· ℬ=0 and ℬ = μℋ = μoμrℋ= μo(1+χff)ℋ = μo(ℋ+ℳ) (2) 0
0 100 200 300 400 500
0.0
0 100 200 300 400 500
Magnetic Field (mT) Magnetic Field (mT)
Where μ= μoμr is the permeability and μr= (1+χff) is the relative
Fig.2. Experimental results showing variation with increasing
permeability of the ferrofluid.
magnetic field (a) POD (b) ARD (c) IDS (d) VOD.
The magnetic body force responsible for droplet deformation in the
However, at the higher flow rate ratio Qr50, there is a decrease in
uniform magnetic field ℋ is defined by [26]
the POD with increasing magnetic field due to the increased drag
𝓕 𝒎 = 𝛻 ∙ 𝜏𝑚 = −(𝓗𝟐 /𝟐)𝛻𝝁 (3)
force from the CP. For cases S1 and S3, which correspond to
Where 𝜏𝑚 = −(𝝁/2)ℋ 2 𝕀 + 𝝁ℋℋ is the magnetic stress tensor
ferrofluids with lower magnetic susceptibility (χ1), variations in the
(indicial form: 𝜏𝑖𝑗 = −(𝜇/2)ℋ 2 𝛿𝑖𝑗 + 𝜇ℋ𝑖 ℋ𝑗 ), “𝕀” is an identity
POD are smaller than that in S2. At lower viscosity (set S1) the POD
matrix [26]. This force only acts on the interface, which is taken into generally decreases with increasing magnetic field at both flow rate
account by the smoothed delta function (δs) [29]. ratios Q1 and Q2. However, at 50 mT, Q1 and at 100 mT, Q2 this
𝓕 𝒎 = −(ℋ 2 /2)𝜇ℎ𝑎𝑟 𝛿𝑠 𝛻𝜙 (4) behavior was not observed. At higher viscosity, lower flow rate ratio
Where μhar is harmonic mean of magnetic permeability of the (set S3Qr10) the POD generally increases with increasing magnetic
medium: 1/(𝜇ℎ𝑎𝑟 ) = (1 − ϵ)/𝜇𝑐𝑝 + ϵ/𝜇𝑑𝑝 field. However, at 25 mT this behavior was not observed. At high flow
3. Drag Force rate ratio (set S3Qr50) the POD increases with increasing magnetic
The drag force on a droplet (radius 𝓇d, viscosity ηdp) in a CP field from 0 to 100 mT. Beyond 100 mT POD decreases and after 250
(viscosity ηcp, velocity 𝓋cp) is given by [30] mT it stabilizes. Evidently, on comparing the POD response at a lower
ℱdd = 6π𝓇d 𝓋cp ηcp (1 + 2ηcp /3ηdp )/(1 + ηcp /ηdp ) (5) flow ratio, high-susceptibility ferrofluid (set S2Qr10) demonstrated
significant changes in the POD with an applied magnetic field
compared to the low susceptibility ferrofluids (set S1Qr10, S3Qr10).
IV. Results and Discussion
Hence, the POD can be more easily controlled by a higher magnetic
We studied the response of the water-based ferrofluid droplets susceptibility, at Qr10 and a lower viscosity of the CP.
under the influence of a magnetic field for different flow rate ratio The effect of magnetic field on the ARD is shown in Fig. 2b. Under
(Q1=10, Q2=50) at a constant Qdp of 10 μl/h and viscosities (η1=3, the influence of magnetic field, droplets elongate along the field
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direction, resulting in a change in the ARD. The magnetic body force
(equation (4)) is responsible for the ARD change. For a high
susceptibility ferrofluid (set S2, Fig. 2b) ARD of the droplets
increases with increasing magnetic field at Qr10 and Qr50. However,
at magnetic fields greater than 50 mT, a significant increase in ARD
is more evident at Qr10 compared to Qr50. This significant increase
in the ARD is due to high magnetic body force for the ferrofluid with
increases with increasing ARD, due to the increase in the magnetic
body force, as discussed earlier. This competition leads to the
increasing VOD with the increase in the Qr, viscosity of the CP and
the POD. Conversely, if the ARD increases, the drag force on the
droplets decreases, resulting in the decrease in the VOD with the
increasing magnetic field strength. However, if the VOD decreases
due to the increasing magnetic field, the IDS decreases.

Dimensionless Droplet Velocity

high magnetic susceptibility, which dominates at Qr10. For low experiment-S1-Qr10
(a) 1.1 experiment-S1-Qr50
experiment-S1-Qr50

Aspect Ratio of Droplets

susceptibility ferrofluids, at Qr10 (set S1Qr10 and set S3Qr10) the simulation-S1-Qr50
1.2 simulation-S1-Qr10
ARD increases with increasing magnetic field from 0 to 100 mT. The simulation-S1-Qr50 1.0
(b)
increases in the ARD stabilizes above 100 mT. At the higher flow rate
ratio of 50 and for low susceptibility (set S1Qr50 and set S3Qr50), the 1.1
0.9
ARD decreases with increasing magnetic field.
This change in the ARD at lower and higher flow rate ratios is the 1.0
0.8
result of the competition between the magnetic body force and the 0 100 200 300 400 500 0 100 200 300 400 500
Magnetic Field (mT) Magnetic Field (mT)
surface tension. At the oil-ferrofluid droplet interface, the magnetic
Fig. 3. Experimental and simulated results of (a) ARD (b)
susceptibility increases in the direction of ferrofluid and decreases in
Dimensionless droplet velocity, defined as vdim=vdrop/vcp.
the direction of the oil phase. The magnetic body force acts at the
From Fig. 2d, the VOD generally increases with increasing
interface where the susceptibility changes. The ARD increases with
magnetic field at Qr50 (set S3Qr50 corresponding to η2χ1Q2).
increasing droplet size (POD) and at a constant uniform magnetic
However, this behavior was not observed at 100 mT. At Qr50 and at
field [27, 31]. The POD for the set S1 at Qr50 (1000 μm) is less than
the higher viscosity, the magnetic drag force dominates, which leads
that at Qr10 (1200 μm). The POD also decreases with increasing
to the velocity increase observed for set S3Qr50. For sets S1Qr50 and
viscosity and increasing magnetic field (Fig. 2a). Hence, the ARD
S2Qr50, the VOD decreases with increasing magnetic field strength
increases with increasing magnetic field at a lower flow rate ratio,
from 10 to 500 mT. Under the influence of the magnetic body force,
lower viscosity and higher susceptibility. At higher flow rate ratio, the
the ARD increases, which reduces the drag on droplets. Hence, the
ARD and the POD both decreases with the increasing magnetic field.
VOD decreases with increasing magnetic field due to the increase in
Figure 3a shows the experimental and simulated results for the
the ARD. There is an anomaly for set S1 at Qr10, where the VOD
ARD versus the magnetic field strength. The simulated and
increases with the increasing magnetic field due to the larger POD at
experimental results of the aspect ratio are in good agreement. The
higher magnetic fields ℋ. The drag force increases with the
simulated results of the ARD for set S1 shows an increasing trend in
increasing POD, hence, the VOD increases with the magnetic field ℋ.
aspect ratio with increasing magnetic field for Qr10. At zero magnetic
Figure 3b shows the variation in the dimensionless velocity of the
field the droplets are spherical. Any change in the shape increases the
droplets (vdim) with the increasing magnetic field strength. The
surface tension. Droplet deformation to an ellipsoidal shape (and with
dimensionless droplet velocity was defined as the ratio of the droplet
an elliptical cross-section) leads to a higher ARD. To maintain this
velocity (vdrop) to the CP velocity (vcp), viz. vdim=vdrop/vcp. Evidently,
non-equilibrium elliptical shape, an external force is required, which
from Fig. 3b for both the experiments and the simulations, the VOD
is supplied by the magnetic volume force [31, 32]. Hence, changes in
decreases with increasing magnetic field strength. Fig. 3b shows good
the surface tension can be correlated to variation in the ARD (Fig. 3a).
agreement between the simulation and the experimental results for the
We determined the surface tension numerically by fitting the
VOD under the influence of a magnetic field ℋ. The observed
experimental ARD to the numerical results [33]. The surface tension
mismatch at 500mT is due to the increase in non-uniformity of the
increases with increasing magnetic field (Fig. 3a) at Qr10 [33].
magnetic fields ℋ (for ℋ equal to or larger than 500 mT).
However, at Qr50 (set S1Qr50 in Fig. 3a), a high ARD was observed
Table 2. Modeled Behavior of χ2 Ferrofluid
at a lower magnetic field of 10 mT, which is below the saturation
magnetization of the ferrofluid. The susceptibility is higher below the Variable X (Magnetic Field)
Sr Variable Y Qr
B≤ 50 mT B > 50 mT
saturation magnetization, resulting in a high magnetic volume force, Droplet 10 Low-ExpDec High-ExpInc
leading to high surface tension (caused by ℋ=10mT), and hence the 1
Perimeter 50 ExpDec Linear Decrease
increased ARD. For magnetic fields above the saturation 2 Aspect Ratio
10 Low-ExpInc High-ExpInc
magnetization of the ferrofluid it follows the usual trend of increasing 50 ExpInc Linear Increase
Droplet 10 Low-ExpDec High-ExpInc
surface tension with increasing magnetic fields at a higher flow rate 3
Spacing 50 ExpInc Linear Decrease
ratio. ExpDec= Exponential Decrease, ExpInc= Exponential Increase. Equation
Figure 2(c and d) shows the variation of IDS and VOD with a Y=1+a⋅X+b⋅cX was used to model (a, b, c are constants).
magnetic field ℋ. The VOD and the IDS changes with increasing
magnetic field. This is a result of competition between the drag force ACKNOWLEDGMENT
acting on droplets (equation (5)), the magnetic body force (equation
(4)) and the surface tension (equation (1)). The drag force increases The authors are grateful to the SERC, Singapore for financial
with increasing viscosity, the velocity of CP and the droplet size (i.e. support for this work through ASTAR PSF 2012 Project: 1321202078.
POD). The magnetic body force increases with increasing magnetic
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