Liquid metals, including eutectic gallium-indium (EGaIn), have been explored for various planar droplet operations, including droplet splitting and merging, promoting their use in emerging areas such as flexible electronics and soft robotics. However, three-dimensional (3D) droplet operations, including droplet bouncing, have mostly been limited to nonmetallic liquids or aqueous solutions. This is the first study of liquid metal droplet bouncing using continuous AC electrowetting through an analytical model, computational fluid dynamics simulation, and empirical validation to the best of our knowledge. We achieved liquid metal droplet bouncing with a height greater than 5 mm with an actuation voltage of less than 10 V and a frequency of less than 5 Hz. We compared the bouncing trajectories of the liquid metal droplet for different actuation parameters. We found that the jumping height of the droplet increases as the frequency of the applied AC voltage decreases and its amplitude increases until the onset of instability. Furthermore, we model the attenuation dynamics of consecutive bouncing cycles of the underdamped droplet bouncing system. This study embarks on controlling liquid metal droplet bouncing electrically, thereby opening a plethora of new opportunities utilizing 3D liquid metal droplet operations for numerous applications such as energy harvesting, heat transfer, and radio frequency (RF) switching.
Liquid metals, including eutectic gallium-indium (EGaIn), have been explored for various planar droplet operations, including droplet splitting and merging, promoting their use in emerging areas such as flexible electronics and soft robotics. However, three-dimensional (3D) droplet operations, including droplet bouncing, have mostly been limited to nonmetallic liquids or aqueous solutions. This is the first study of liquid metal droplet bouncing using continuous AC electrowetting through an analytical model, computational fluid dynamics simulation, and empirical validation to the best of our knowledge. We achieved liquid metal droplet bouncing with a height greater than 5 mm with an actuation voltage of less than 10 V and a frequency of less than 5 Hz. We compared the bouncing trajectories of the liquid metal droplet for different actuation parameters. We found that the jumping height of the droplet increases as the frequency of the applied AC voltage decreases and its amplitude increases until the onset of instability. Furthermore, we model the attenuation dynamics of consecutive bouncing cycles of the underdamped droplet bouncing system. This study embarks on controlling liquid metal droplet bouncing electrically, thereby opening a plethora of new opportunities utilizing 3D liquid metal droplet operations for numerous applications such as energy harvesting, heat transfer, and radio frequency (RF) switching.
Room temperature liquid
metals have gained significant attention
with their numerous applications for soft robotics and flexible electronics
such as micro-electro-mechanical system (MEMS) switches,[1] haptic and visual displays,[2,3] reconfigurable
radio frequency (RF) systems,[4] and many
others.[5] Liquid metals have unique properties
of low viscosity, high thermal and electrical conductivity, and large
surface tension, which support the active manipulation of droplets
using an electric field.[6] The electrically
induced liquid oscillations for conductive and dielectric nonmetallic
liquid droplets have been researched for multiple decades;[7−9] however, effective electrical manipulation of liquid metals originated
with the discovery of continuous electrowetting (CEW).[10] Electrowetting has been explored with various
liquid metals,[11] including aluminum,[12] gallium,[13] and mercury.[14] Eutectic gallium–indium alloy (EGaIn)
has emerged as one of the most viable liquid metals because of its
extraordinary properties such as excellent fluidity, low melting point,
high conductivity, and low toxicity, marking it a promising candidate
for applications such as flexible electronics,[15] microfluidic acoustic metamaterials,[16,17] and conductive printing.[18] The electrowetting
of EGaIn has also been researched by controlling the surface tension
of the liquid metal for active droplet manipulation.[3,18,20] However, the electrowetting actuation
of liquid metals is to date limited to the in-plane manipulation of
a droplet on an electrically controlled substrate.[20−22] Recently, liquid
metal droplet jump from a surface has been explored using electrochemical
surface reactions[23] and by the contact
of solid metal particles with liquid metal droplets in an electrolyte
solution.[24] Liquid metals coated with nanoparticles,
called liquid metal marbles, have also been actuated electrochemically
to realize opportunities for flexible liquid electronics, superstructures,
and other unusual mechanical properties.[25] However, to the best of our knowledge, the bouncing dynamics of
a liquid metal droplet using electrical actuation have never been
reported. Here, for the first time, we investigate the electrically
induced bouncing dynamics of liquid metal droplets actuated by AC
continuous electrowetting both experimentally and by simulation.For the aqueous solution or nonmetallic liquid droplets, the jumping
motion using AC electrowetting has been explored for applications
in three-dimensional (3D) digital microfluidics,[26,27] and numerical models have been developed for both jumping and bouncing
processes.[28] Various studies have been
reported on the bouncing of aqueous droplets on different substrates,
such as microstructured superhydrophobic surfaces without an electric
field[29,30] and topographically structured surfaces
with an electric field,[31] to analyze the
impact of gravity, impact velocities, and substrate geometries. Energy-based
models have also been utilized to examine the dynamical process of
rebounding and adhesion of water droplets on hydrophobic surfaces.[32,33] Moreover, the shape-dependent dynamics of a bouncing ellipsoidal
drop on a superhydrophobic surface have also been investigated and
reported to reduce the contact time and bouncing magnitude of droplets.[34] It has been observed that the vertical jumping
motion of aqueous solution droplets generally requires high voltage
(>50 V) and can be achieved with minimal loss during the resonance.[35,36] Thus, the droplet bouncing behavior depends on multiple factors
such as the substrate roughness, hydrophobicity, liquid properties
(surface tension and viscosity), ambient surrounding liquid, applied
voltages, and frequencies.The present study investigates a
liquid metal (EGaIn) droplet bouncing
in sodium hydroxide (NaOH) solution using continuous electrowetting
for different actuation parameters, namely, the AC voltage amplitudes
and frequencies. The key contributions of this study are as follows:
(1) We achieve a high jump of the liquid metal droplet (∼6
mm) from a normal flat surface in a viscous solution (more viscous
than air) by applying less than 10 V voltage, far lower than the previously
reported voltages (50–100 V) to drive the droplet jumping from
a superhydrophobic surface in the air, which is induced using an electrowetting-on-dielectric
(EWOD) technique.[35,36] (2) In addition to the experimental
studies, we also simulate the liquid metal droplet bouncing and oscillation
using computational fluid dynamics (CFD), to provide a systematic
approach for prototyping future applications. (3) We analyze the liquid
metal droplet bouncing dynamics, involving temporal changes in the
center of mass of the droplet, droplet jump height, and contact length,
for different actuation parameters (voltages and frequencies) of AC
electrowetting. We establish that the droplet jumps higher with an
increase in AC voltage amplitude and decrease in frequency, until
the onset of instability. (4) We model the attenuation dynamics of
bouncing cycles of the liquid metal droplet in analogy to a mechanical
damped harmonic (mass–spring–damper) oscillator system.
Materials and Methods
Experimental Setup
For the experimental study, clear
acrylic sheets were laser-cut and bonded with a UV-curing resin to
create a rectangular bath for the NaOH solution (as shown in Figure A). The acrylic (PMMA)
is resistant to NaOH solution, and the transparency of the bath allowed
the experiment to be filmed using a high-speed camera with enough
background light, as shown in Figure C. A small hole was cut into the base of the bed, and
a silver-plated wire (diameter of 0.2 mm) was inserted as a working
electrode. The electrode wire was stuck into liquid metal droplets
to constantly supply current to the liquid metal during bouncing and
the horizontal shift of the droplet was limited. Another silver wire
electrode was positioned at the corner of the NaOH bath as a counter
electrode. An Arduino Uno microcontroller board was used to generate
a square wave with different frequencies. An L293D dual H-bridge motor
driver was connected to the Arduino digital output, and a regulated
DC power supply (Mastech HY1803D) to support a square wave for driving
AC continuous electrowetting up to 600 mA of the maximum current was
used.
Figure 1
Experiments of continuous electrowetting with the EGaIn liquid
metal droplet. (A) Experimental image of a liquid metal droplet in
NaOH solution with wire electrodes. (B) Young–Lippmann curve
plotting the change in the contact angle of the droplet with the applied
DC voltage. (C) Schematic illustration of the experimental setup to
record the bouncing motion of the EGaIn droplet actuated by AC continuous
electrowetting.
Experiments of continuous electrowetting with the EGaIn liquid
metal droplet. (A) Experimental image of a liquid metal droplet in
NaOH solution with wire electrodes. (B) Young–Lippmann curve
plotting the change in the contact angle of the droplet with the applied
DC voltage. (C) Schematic illustration of the experimental setup to
record the bouncing motion of the EGaIn droplet actuated by AC continuous
electrowetting.
Choice of Materials
Eutectic gallium–indium
(EGaIn) liquid metal alloy, comprising 75% gallium and 25% indium,
was used for the continuous electrowetting experiments and simulations.
An EGaIn droplet of 23 ± 4 μL volume (diameter of 3.6 ±
0.2 mm), 1.99 × 10–3 Pa·s[6] bulk viscosity, and 509 mN/m[2,19] surface tension
was placed in a sodium hydroxide (NaOH) solution bath. NaOH (1M) was
used as an electrolyte to create a basic pH environment that dissolves
the surface oxide of the liquid metal,[37] which would otherwise interfere with the wetting dynamics and contact
angle.[38] The dissolution of gallium oxide
proceeds through the following reaction[39]EGaIn was preferred to other liquid metals
in this study for the following reasons: (1) EGaIn is nontoxic; (2)
the melting point of EGaIn (15.7 °C) is lower than standard room
temperature, and so the metal remains in its liquid state, providing
ease to conduct the experiments; and (3) it is highly conductive (2.94
× 10–8 Ω·m),[40] having a resistivity lower than that of gallium (14 ×
10–8 Ω·m) and mercury (90.9 × 10–8 Ω·m). The properties of EGaIn and other
liquid metals are summarized in Table for comparison.
Table 1
Properties of Different
Liquid Metals
mercury (Hg)
field’s
metal (BiInSn)
gallium (Ga)
gallium–indium (EGaIn)
melting point (°C)
–38.83
62
29.76
15.7
toxicity
high
low
low
low
electrowetting
applicable
N/A
applicable
applicable
resistivity (Ω·m)
90.9 × 10–8
52 × 10–8
14 × 10–8
2.94 × 10–8
Resonant Frequency
The resonant
frequency (ω)
of a freely oscillating liquid droplet for the nth
mode oscillation is given as[41−43] ω2 = (σLVn(n – 1)(n + 2)/ρ)q3, where σLV is the interfacial tension of the liquid metal and surrounding
electrolyte interface, n is the mode number, ρ
is the density of EGaIn, and q is the characteristic
length of the droplet. The resonant frequency of the actuated EGaIn
droplet (q = 1.8 mm) is ∼55 Hz approximately.
Experimental Procedure
For the initial DC electrowetting
experiment, we used 0–2 V DC voltage to measure a change in
the droplet contact angle with voltage, and the Young–Lippmann
curve was plotted as shown in Figure B. For the AC electrowetting experiment, we applied
a 4–9 V (in the step of 1 V) square wave with frequencies of
0.5, 1, 2, and 4 Hz. The experiment was conducted five times for each
set of voltage and frequency. The droplet bouncing motion caused by
AC electrowetting was recorded with a high-speed camera (Photron FASTCAM
Nova S6 type 800K-M-32GB) at a frame rate of 2000 frames per second,
as shown in Figure C. The contact angle was measured from the captured images using
ImageJ software. The dynamic change in contact length (i.e., the base
diameter of the droplet in contact with the substrate) and the height
of the center of mass of the droplet from the ground surface was analyzed
with our custom-made image-processing pipeline based on the OpenCV
library written in Python.
Results and Discussion
Young–Lippmann
Curve
Electrocapillarity,[44] proposed
by Lippmann,[45] controls the surface energy
of liquid metals by changing the electrical
potential between electrodes in an electrolytic solution. Continuous
electrowetting of liquid metal droplets is based on the same principle
and electrically controls the wetting properties of a liquid–solid
interface and the liquid–liquid interface.[46,47] The movement of liquid metal droplets driven by an electric field
has been modeled based on electrowetting and electrocapillarity theory.[48] Young’s equation defines the relationship
of interfacial energies with the equilibrium contact angle (θY) as[49], where three interfacial tensions are considered
between the liquid droplet and the solid substrate (σSL), the solid substrate and the surrounding medium (σSV), and the liquid droplet and the surrounding medium (σLV).The Lippmann equation describes the change in the
effective interfacial tension (dσSLeff) with the change
in voltage (dU) aswhere φSL is the surface
charge density. There is no insulator between the droplet of EGaIn
and the metal electrode; however, an electrical double layer (EDL)
builds upon the boundary between the droplet and the surrounding sodium
hydroxide solution (NaOH). The capacitance of this layer can be calculated
as , where dH is
the thickness of the electrical double layer (EDL) (generally <10
nm[50−52]). Thus, for an applied voltage (U), the interfacial
tension is given aswhere UPZC is
the voltage potential of zero charge and σSL0 is the interfacial tension between
the droplet and the solid substrate at zero electric field. By combining
Young’s and Lippmann’s equations, we get the Young–Lippmann
equation aswhere is the electrowetting number, is the capacitance per unit area, Ueff = U – UPZC is the effective voltage potential, θY is the Young equilibrium contact angle, and θ is the equilibrium
apparent contact angle of electrowetting after applying voltage. The
Young–Lippmann curve showing the change in the contact angle
of the liquid metal droplet with the voltage is plotted in Figure B.
Computational
Fluid Dynamics Simulation
We used COMSOL
Multiphysics 5.3 software to model the actuation of a liquid metal
droplet with continuous electrowetting. We built a two-dimensional
(2D) axisymmetric laminar two-phase flow model to simulate a liquid
metal droplet’s deformation and bouncing motion using computational
fluid dynamics (CFD). The central axis of the 2D axisymmetric model
was set along the working electrode. The Navier–Stokes equation
with the level set method was used to determine the liquid metal flow
and measure the deforming boundary of an immiscible interface between
the EGaIn and NaOH electrolyte solution. The base and outer boundaries
of the NaOH solution bath were modeled as solid boundaries, and the
top boundary was set as a liquid–air interface. A fine dynamic
mesh (14 triangle meshes/mm) was used around the boundary of the liquid
metal droplet to precisely model the dynamical liquid metal surface
movement, while a coarser mesh (11 triangle meshes/mm) was used toward
the more static region of the NaOH solution. A total number of 16,379
mesh elements were used in the entire simulation domain (5 mm ×
10 mm).We first examined the accuracy of our electrowetting
actuation model for an EGaIn droplet (23 μL) with multiple DC
voltages. We supplied the DC voltage to the working electrode wire
in the range from 0 to 2 volts with a step of 0.2 V, where 0.2 s intervals
were set to allow enough time for the EGaIn droplet to deform. We
measured the contact angle of the liquid metal droplet at each voltage
and plotted the Young–Lippmann curve (Figure B). We observed that the simulation model
and experimental values show a good agreement. Utilizing the same
electrowetting actuation model and experimental setup, we examined
the EGaIn droplet bouncing by applying AC square voltages with multiple
amplitudes and frequencies in both simulations and experiments. We
investigated the voltage range from 4 to 9 V with a step of 1 V. Figure shows the captured
images of the bouncing droplet at the maximum stretch states and the
maximum jump states, when a 23 μL EGaIn droplet was actuated
by a 5 V square wave with a frequency of 0.5 Hz. Experimental results
(left-half droplet) and simulation model outputs (right-half droplet)
for each time frame show good agreement for the electrically induced
bouncing motion of the droplet.
Figure 2
Image instants for four different time
frames during electrically
induced bouncing of the liquid metal droplet by both experiments and
simulations. At each captured time frame, the (left-half) experimental
and (right-half) simulated half droplet images are shown in the left
and right quadrant in parallel, respectively. A 23 μL EGaIn
droplet was actuated using AC electrowetting with a 5 V square wave
at a frequency of 0.5 Hz. The images were captured at time frames
when the first and second maximum deformations and the maximum jump
height were achieved [Supporting Information Videos].
Image instants for four different time
frames during electrically
induced bouncing of the liquid metal droplet by both experiments and
simulations. At each captured time frame, the (left-half) experimental
and (right-half) simulated half droplet images are shown in the left
and right quadrant in parallel, respectively. A 23 μL EGaIn
droplet was actuated using AC electrowetting with a 5 V square wave
at a frequency of 0.5 Hz. The images were captured at time frames
when the first and second maximum deformations and the maximum jump
height were achieved [Supporting Information Videos].
Droplet Bouncing Dynamics:
Experiments and Simulations
The electrically induced bouncing
process can be classified into
five stages as shown in Figure A: (I) an EGaIn droplet is at rest, initial unactuated state;
(II) the droplet spreads when a positive voltage is applied to the
droplet; (III) retraction occurs when the applied voltage drops to
zero because of the increase in interfacial tension; (IV) the droplet
recoils along the working electrode as the droplet momentum shifts
from the horizontal axis to the vertical axis; and (V) the droplet
is detached from the surface with an excessive amount of momentum[27] and bounces in the electrolyte solution until
the momentum drops to zero due to the force of the gravity.
Figure 3
Electrically
induced bouncing dynamics of the droplet. (A) Process
state transition diagram of actuated liquid metal: (I) Initial unactuated
state, (II) spread state when the voltage is applied, (III) retract
state when the voltage drops to zero, (IV) recoil, and (V) jump. (B)
Superimposed experimental images of the droplet during different bouncing
cycles upon actuation with 5 V voltage at 0.5 Hz frequency. (C) Time
evolution of the average height (mm) of the center of mass of a bouncing
droplet. The red line shows an experimental result, and the black
line shows a simulation output when a 5 V square wave is applied with
a frequency of 0.5 Hz. (D) Complementary relationship of the height
(mm) of the center of mass (black) and the contact length of the droplet
(blue) from the simulation (i.e., when one increases, the other decreases).
Electrically
induced bouncing dynamics of the droplet. (A) Process
state transition diagram of actuated liquid metal: (I) Initial unactuated
state, (II) spread state when the voltage is applied, (III) retract
state when the voltage drops to zero, (IV) recoil, and (V) jump. (B)
Superimposed experimental images of the droplet during different bouncing
cycles upon actuation with 5 V voltage at 0.5 Hz frequency. (C) Time
evolution of the average height (mm) of the center of mass of a bouncing
droplet. The red line shows an experimental result, and the black
line shows a simulation output when a 5 V square wave is applied with
a frequency of 0.5 Hz. (D) Complementary relationship of the height
(mm) of the center of mass (black) and the contact length of the droplet
(blue) from the simulation (i.e., when one increases, the other decreases).We captured different bouncing cycles of the liquid
metal droplet
with a high-speed camera, and a few superimposed droplet images for
electrowetting actuation with a 5 V square wave of 0.5 Hz frequency
are shown in Figure B. To track the time evolution of the bouncing motion, we captured
the trajectory of the center of mass of the liquid metal droplet using
the OpenCV-Python image-processing pipeline. We recorded the height
of the center of mass and contact length of the droplet on the ground
plane by detecting the droplet as a blob in a binary-processed image.
The experimental result (red line) and the simulation model (black
line) show good agreement, as shown in Figure C.We also measured the contact length
of the droplet and found that
it increases with the decrease in the height of the center of mass
(i.e., the jump height), as shown in Figure D. This result supports the complementary
relationship of the jump height and contact length, as a liquid metal
droplet conserves the momentum in horizontal spreading motion and
vertical jumping motion.We empirically studied the droplet
bouncing dynamics actuated by
AC electrowetting with a square wave voltage ranging from 4 to 9 V
with a step of 1 V and frequency of 0.5, 1, 2, and 4 Hz. The time
evolution of the height of the center of mass of the droplet for different
voltages is plotted in Figure A–D. For every frequency, we observed that the maximum
height of the droplet in the first bouncing cycle increased as the
applied voltage was increased. This is because an increase in the
applied voltage leads to a more spread droplet area with a larger
droplet contact length. Thus, when the applied voltage drops to zero,
the droplet gains more kinetic energy as it retracts from the more
spread state due to the higher voltage input. Since the kinetic energy
of the droplet is converted into the gravitational potential energy
in the recoiling stage, a larger jump height is achieved by a higher
voltage. However, we observed that the jump height decreased above
7 V for some frequencies. This is attributed to an instability causing
satellite droplets and electrolysis bubbles around the surface of
the droplet for electrowetting at above 7 V (i.e., 8 and 9 V input
voltages). Faradaic reactions are caused at the boundary of liquid
metal/electrodes and NaOH electrolyte at high electrowetting voltages,
which causes electrolysis and generates bubbles of oxygen or hydrogen
depending on whether the potential applied to the liquid metal is
positive (oxidizing) or negative (reducing), respectively.[39]
Figure 4
Bouncing trajectories of the center of mass of the EGaIn
droplet
by CEW actuation at different voltages and frequencies. (A–D)
Temporal behavior of the center of mass of the droplet launched with
a square wave of different applied voltages (4–9 V in the step
of 1 V) at frequencies of 0.5, 1, 2 and 4 Hz, respectively. (E, F)
Maximum jump height for (E) first bouncing cycle and (F) second bouncing
cycle of the liquid metal droplet upon actuation with the CEW at different
voltages and frequencies.
Bouncing trajectories of the center of mass of the EGaIn
droplet
by CEW actuation at different voltages and frequencies. (A–D)
Temporal behavior of the center of mass of the droplet launched with
a square wave of different applied voltages (4–9 V in the step
of 1 V) at frequencies of 0.5, 1, 2 and 4 Hz, respectively. (E, F)
Maximum jump height for (E) first bouncing cycle and (F) second bouncing
cycle of the liquid metal droplet upon actuation with the CEW at different
voltages and frequencies.The partial equations for electrolysis of water are as follows:At the anode (positive
electrode),
the oxygen anions are oxidized when they lose electrons: 2H2O → O2 + 4H+ + 4e–.At the cathode (negative
electrode),
the hydrogen cations are reduced when they gain electrons: 2H2O + 2e– → H2 + 2OH–.Hence, the net reaction
of the electrolysis is 2H2O
→ 2H2 + O2.The instability reduces
the kinetic energy of the liquid metal
droplet and lowers the maximum jump height, as shown in Figure E,F. The maximum height observed
in these experiments is 6 mm, which is less than the theoretical value
of 14.6 mm reported in the literature,[23] due to the unaccounted system losses such as viscous drag and viscoelastic
dissipation.The driving frequency also affected the maximum
height of the droplet
center of mass and the following bouncing heights, as shown in Figure . We observed that
as the applied frequency increased from 0.5 to 4.0 Hz, both the maximum
jump height and subsequent bouncing height decreased. This is because
as the frequency of electrowetting actuation increases, the time available
for the droplet to spread on the ground decreases, and consequently,
the droplet gains less kinetic energy to jump.
Effect of Droplet Size
With the applied voltage, the
base radius also increases until saturation, thereby leading to an
increase in the surface area (ΔA). The excess
interfacial surface energy (ΔES)
is related to the potential energy (ΔEP) as σLV ΔA = ρghVl where g is the gravitational
constant, Vl is the droplet volume, and h is the jumping height.[23] Thus,
the ratio of change in the surface area (ΔA) to the droplet volume (Vl) affects
the droplet bouncing dynamics. The droplet bouncing through droplet
coalescence or impact collisions is promoted by increasing the droplet
diameter but suppressed by decreasing it.[53] In these cases, by increasing the droplet diameter, the Ohnesorge
number, i.e., the ratio of viscous forces to the inertia and surface
tension forces, decreases and enhances the bouncing dynamics.[31,54]
Energy Cycle
The droplet bouncing process involves
multiple energy conversion cycles, as shown in Figure . First, the interfacial tension of the liquid
metal–electrolyte interface decreases due to the applied electric
field. This decrease in interfacial tension causes the droplet to
spread to balance the interfacial energies (Es). The surface energy is given aswhere σLV, σSL, and σSV are the
three interfacial tensions and ALV, ASL, and ASV are
the surface areas for the liquid droplet
and the surrounding medium interface, the liquid droplet and the solid
substrate interface, the solid substrate and the surrounding medium
interface, respectively.
Figure 5
Schematic showing mechanical analogy of (A)
simple damped harmonic
oscillator (mass–spring–damper system) and (B) liquid
metal underdamped droplet bouncing system.
Schematic showing mechanical analogy of (A)
simple damped harmonic
oscillator (mass–spring–damper system) and (B) liquid
metal underdamped droplet bouncing system.Subsequently, when the electric field (and electrowetting force)
is removed, the interfacial tension increases and retracts the droplet
to its initial minimum surface energy state. In the retraction stage,
the surface energy stored during electrowetting is converted into
kinetic energy (ΔEK), stated as
ΔEK = 1/2 ρVl (2πfa)2, where ρ
is the density of EGaIn, f is the actuation frequency,
a is the amplitude of droplet motion, (2πfa) is the speed of the moving EGaIn droplet, and Vl is the volume of the droplet (23 μL).When
the total energy of the droplet, i.e., the sum of instantaneous
surface energy and kinetic energy, exceeds the initial surface energy
of the droplet, the excess amount of energy makes the droplet jump.
Subsequently, assuming that the excess interfacial surface energy
(ΔES) is entirely converted into
the gravitational potential energy (ΔEP = ρghVl) and causes the
droplet to bounce off the ground surface, we get σLV ΔA = ρghVl, where g is the gravitational constant, ΔA is the difference in the surface area of the liquid metal
at the spread state and the unactuated state, and h is the jumping height. The upper limit of jumping height using this
expression was determined to be 14.6 mm.[23] The bouncing motion attenuates because of the energy loss incurred
by the viscoelastic damping force, drag force from the surrounding
medium, and inelastic collisions of the droplet on the substrate.
The liquid metal droplet stabilizes to the equilibrium position after
a few bouncing cycles. Then, it restarts from the initial unactuated
electrowetting stage and repeats the same energy cycle to attain a
bouncing motion. The dynamical change in interfacial tension that
determines the bouncing behavior of a liquid metal droplet can be
controlled by the magnitude and frequency of the applied voltage through
AC continuous electrowetting.
Mass–Spring–Damper
Model
We model the
attenuation dynamics of a series of underdamped droplet bouncing cycles
in analogy to a simple damped harmonic oscillator (mass–spring–damper
model[55]), as shown in Figure . The droplet bouncing system
is driven by the imbalance of interfacial tension energies, droplet
kinetic energies, and potential energies after the electrowetting
force is removed (i.e., the actuation voltage drops to 0 V). The spring–mass–damper
model used to fit the bouncing cycles also depends on the actuation
parameters, which lead to different bouncing heights of the droplet,
contact lengths, and contact time durations. A general bouncing motion
of a liquid metal droplet can be classified into two motion regimes:[55] free flight motion and underdamped oscillation
motion.If the initial jump height driven by electrowetting
is high enough, the liquid metal droplet lifts off the substrate and
follows free flight motion where the contact length becomes zero as
shown in Figure D.After colliding the substrate (contact length > 0), the liquid
metal droplet undergoes underdamped bouncing motion till the center
of mass of the liquid metal stabilizes to the equilibrium position
where the gravity force on the liquid metal is balanced by the interfacial
tension of the liquid metal and the substrate.We applied a
piecewise mass–spring–damper model[55] to realize both free flight motions and underdamped
oscillation motions of bouncing droplets based on the contact state
with the substrate [details in the Supporting Information]. The trajectory of the ith bouncing
cycle, which consists of the free flight motion (y1(t)) and the underdamped
oscillation motion (y2(t)), is expressed based on the condition of liquid
metal contact length (L) at the substrate as followswhereand t1 is the time when the liquid
metal is detached from the substrate
and t2 is the time when
the liquid metal hits the substrate in the ith bouncing
cycle.The model fits the bouncing dynamics of the experimental
data,
as shown for the case when the liquid metal was actuated by 5 V voltage
at 0.5 Hz frequency in Figure A. The initial conditions of the height and speed of y1 (t) and y2 (t) in
the bouncing cycles were calculated from the continuity of the free
flight motion and the underdamped oscillation motion at the transition
time (i.e., t1 and t2). The initial speed and
the height of the flight motion of the first cycle were given by the
experimental data at the time t11 = 7
ms, when the liquid metal was observed to lift off the substrate after
the release of the electrowetting force (i.e., contact length becomes
zero for the first time in Figure D). The transition time of each cycle was measured
from the experimental data when the contact length (L) is switched between zero and positive values in Figure D.
Figure 6
(A) Bouncing motion of
the liquid metal droplet by electrowetting
actuation at 5 V and 0.5 Hz frequency. The black curve plots the experimental
data, and the blue curve plots the piecewise bouncing model. (B) Decay
constant of the underdamped droplet bouncing cycles by electrowetting
at different voltages and frequencies.
(A) Bouncing motion of
the liquid metal droplet by electrowetting
actuation at 5 V and 0.5 Hz frequency. The black curve plots the experimental
data, and the blue curve plots the piecewise bouncing model. (B) Decay
constant of the underdamped droplet bouncing cycles by electrowetting
at different voltages and frequencies.The root-mean-square deviation (RMSD) of the model from the experimental
result is 0.05 mm.Since the first and second bouncing cycles
in Figure A (i.e.,
7 ≤ t < 126.5 ms) include the high free
flight motion, the
large momentum of the falling liquid metal leads to the deviation
of the underdamped oscillation motion model from the experimental
result with the RMSD of 0.08 mm. From the third bouncing cycle (i.e., t ≥ 126.5 ms), the impact of the free flight motion
on the underdamped oscillation motion becomes negligible due to the
decay of the jump height, and the mass–spring–damper
model accurately expresses the attenuation of the bounce until the
liquid metal stabilizes to the equilibrium position with the RMSD
of 0.02 mm.With a simplified mass–spring–damper
model, the underdamped
bouncing of the liquid metal droplet can be expressed by mÿ + cẏ + ky = mg, where k is a spring constant, c is a damping coefficient, m is a mass of the liquid
metal droplet, g is the gravitational constant, and y is the displacement of the center of mass of the liquid
metal from the substrate. The damping coefficient (c) is equivalent to the viscous damping coefficient of the moving
EGaIn droplet in the NaOH electrolyte solution, and the spring constant
(k) is comparable to the interfacial tension between
the substrate and liquid metal (σLV ∼ k).An exponentially decaying solution for the underdamped
harmonic
oscillator equation is given as follows[56]where y0 is the
equilibrium position when the liquid metal droplet remains at rest
without electrowetting (i.e., ky0 = mg).We determined the peak height values (yp) of each bouncing cycle from the plotted trajectories
of the center
of mass of the bouncing droplet (Figure ). We fit the measured peak values in an
exponential curve equation, yp(t) = α exp(−βt) + y0, to determine the decay constant
(β) of the underdamped harmonic oscillator model.[57] The power of the fitted curve (β) is expressed
by c/2m as shown in the equation
given above. We calculated the decay constants of the system for different
voltages and frequencies to analyze the attenuation dynamics in a
series of bouncing cycles. The decay constant of the underdamped bouncing
cycles increases as the amplitude of the applied AC voltage and its
frequency increases, as shown in Figure B. This implies that the bouncing motion
fades faster with larger voltage and frequency.
Conclusions
Dynamical actuation of high-density liquid metals against gravity
can revolutionize multiple sectors with applications ranging from
3D microfluidics to energy harvesting. While the vertical bouncing
motion of nonmetallic droplets has been well investigated by the AC
electrowetting actuation method, the same phenomenon has rarely been
reported for liquid metal droplets. Here, we investigated the electrically
induced bouncing motion of a liquid metal droplet using less than
10 V voltage and low-frequency AC continuous electrowetting. We explored
the bouncing dynamics of eutectic gallium–indium alloy (EGaIn)
droplets for different driving frequencies and voltages of an AC square
wave. We achieved droplet bouncing at voltages (<10 V) and frequencies
(≤4 Hz) that are far lower than the resonant frequency of the
droplet (55 Hz). AC continuous electrowetting actuation allows a droplet
to bounce from a non-superhydrophobic surface in more viscous medium
than the air. We investigated the droplet bouncing dynamics by both
the CEW experiments and CFD simulations and analyzed the effect of
the applied AC voltage amplitudes and frequencies on the droplet bouncing
trajectories. The maximum droplet jump height was found to increase
with an increase in voltage and decrease in frequency until we observed
an instability such as the formation of satellite droplets or electrolysis.
The bouncing motion tends to fade out slowly because the energy is
lost by the inelastic collision of the droplet with the substrate
and by viscous drag through the electrolyte solution. We explained
the electrically induced droplet bouncing motion based on energy conversion
cycles and modeled the attenuation of consecutive bouncing cycles
using a mass–spring–damper model. Our experimental results
show that the decay constant of the underdamped bouncing cycles increases
with an increase in voltage and increase in frequency. This study
about the electrical control of liquid metal droplet bouncing using
a facile AC electrowetting technique can open a plethora of applications
such as 3D digital microfluidics,[58] RF
switching,[1] energy harvesting,[59] portable lab-on-a-chip applications,[60] and heat transfer systems.[61]
Authors: Mohammad Rashed Khan; Collin B Eaker; Edmond F Bowden; Michael D Dickey Journal: Proc Natl Acad Sci U S A Date: 2014-09-16 Impact factor: 11.205