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Mohamed Maher
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© © All Rights Reserved
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SCIENCE ADVANCES | RESEARCH ARTICLE

PHYSICS Copyright © 2019


The Authors, some

Final fate of a Leidenfrost droplet: Explosion or takeoff rights reserved;


exclusive licensee
American Association
Sijia Lyu1*, Varghese Mathai2*, Yujie Wang1, Benjamin Sobac3, Pierre Colinet3, for the Advancement
Detlef Lohse1,4, Chao Sun1,4† of Science. No claim to
original U.S. Government
When a liquid droplet is placed on a very hot solid, it levitates on its own vapor layer, a phenomenon called the Works. Distributed
Leidenfrost effect. Although the mechanisms governing the droplet’s levitation have been explored, not much is under a Creative
known about the fate of the Leidenfrost droplet. Here we report on the final stages of evaporation of Leidenfrost Commons Attribution
droplets. While initially small droplets tend to take off, unexpectedly, the initially large ones explode with a crack NonCommercial
sound. We interpret these in the context of unavoidable droplet contaminants, which accumulate at the droplet- License 4.0 (CC BY-NC).
air interface, resulting in reduced evaporation rate, and contact with the substrate. We validate this hypothesis
by introducing controlled amounts of microparticles and reveal a universal 1/3-scaling law for the dimensionless
explosion radius versus contaminant fraction. Our findings open up new opportunities for controlling the dura-
tion and rate of Leidenfrost heat transfer and propulsion by tuning the droplet’s size and contamination.

INTRODUCTION RESULTS

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For a droplet deposited on a heated substrate, the evaporation rate The experiments were performed with droplets placed on a heated
generally increases with the temperature of the substrate. But when quartz substrate (see Fig. 1A). Side-view recordings were used to mea-
the temperature is above a certain value, the droplet levitates on its sure the radius, elevation, and state of droplets, while bottom-view
own vapor layer, and the evaporation rate markedly reduces because images served to distinguish levitation from contact with the substrate.
of the poor heat conductivity of the vapor layer. This effect, known as We found two markedly different behaviors at the final evaporation
the Leidenfrost effect (1, 2), while highly undesirable in certain cooling stage (see Fig. 1, B and C), with the same temperature of the substrate
applications (3), can be of great use in many industrial processes, for (Ts = 296°C). When a “pure” ethanol droplet (pure droplet means a
example, in chemical reactors without borders (4), in frictionless cleanly prepared droplet that meets the analytical reagent standards
transport of small electronic compounds (5), in propelling droplets for purity) of small initial radius, Ri ≈ 30 mm, is placed on the hot sub-
in preferred directions (6–8), and in drag reduction using the vapor strate, it first drops down to a lowest location without contacting the
layer (9, 10). As the vapor layer between the levitating droplet and substrate and then spontaneously takes off (see Fig. 1B). The lower
the substrate is of prime importance to the Leidenfrost phenomena, plot (Fig. 1D) shows the measured levitation height versus time, where
a vast number of studies have been conducted on its characteristics the droplet reaches a minimum height h ≈ 50 mm. In contrast, when
(2, 11–13). These have yielded a clear understanding of both the dy- the droplet’s initial radius is larger, it stably levitates on a vapor layer
namic and quasi-steady aspects of Leidenfrost droplets (14, 15). and finally explodes (see Fig. 1C). A microphone was synchronized
However, comparatively little attention has been paid to the final with the high-speed camera. In all experiments, the “crack” sound
stages of evaporation of Leidenfrost droplets. One of the few investi- was heard (Fig. 1E) when the explosion occurred, similarly as reported
gations is due to Celestini et al. (16), who conducted experiments with by Leidenfrost (1). The same two final fates were observed for a variety
small Leidenfrost droplets of water and ethanol. They reported that of pure liquids, including ultrapure water, ethanol, methanol, butanol,
when the evaporating droplet becomes smaller than a well-defined ra- acetone, and hydrofluoroethers (Novec 7000 and Novec 7100 from
dius, it suddenly takes off from the substrate, reaching an elevation 3M Ltd.).
much higher than its radius, before it finally disappears. This phenom- From the above observations, it seems that the initial size of the
enon was also observed on substrates below the Leidenfrost tempera- droplet has an important role in the final Leidenfrost dynamics. We
tures (17), where water droplets were found to evaporate down to a hypothesize that the possible reason for the two different final out-
critical size and then rapidly rise away. But do all Leidenfrost droplets comes is the amount of solid contaminants present within the drop-
ultimately take off from the substrate? Here, we study the final stages let. In general, even with the most careful preparations, no droplet is
of evaporation of droplets on very hot substrates. We observe the ex- perfectly pure, but inevitably contains small amounts of contamina-
istence of two final fates for evaporating Leidenfrost droplets: one that tion. For the pure droplets in our experiments, the volume fraction of
leads to droplet explosion and the other resulting in droplet takeoff contaminants is extremely low [~1 part per million (ppm) (18)]. Yet,
(16). We explain how the physical reason for the two final fates (ex- one can speculate that when a sufficiently large pure droplet evapo-
plosion versus takeoff) lies in the minute amounts of contamination rates, this small amount of contaminants within the drop can accu-
within the droplets, and provide a predictive criterion to determine the mulate at the droplet interface, thereby modifying its Leidenfrost
final state in terms of the initial conditions of the droplet. dynamics (19, 20).
While one cannot make ethanol purer, an easier route to test our
1
hypothesis is to make the droplet dirtier. We added controlled amounts
Center for Combustion Energy, Key Laboratory for Thermal Science and Power
Engineering of Ministry of Education, Department of Energy and Power Engineering,
of hydrophilic rutile titanium dioxide (TiO2) microparticles into large
Tsinghua University, 100084 Beijing, China. 2School of Engineering, Brown Univer- ethanol droplets (21). The particles have a radius Rp ≈ 1 mm, which is
sity, Providence, RI 02912, USA. 3Université libre de Bruxelles, TIPs-Fluid Physics, comparable in size to typical contaminants present in pure liquid
1050 Brussels, Belgium. 4Physics of Fluids Group and Max Planck Center Twente sample (18, 22). In the experiments, we independently vary the initial
for Complex Fluid Dynamics, University of Twente, Enschede, Netherlands.
*These authors contributed equally to this work. amount of particles fi, the substrate temperature Ts, and the initial
†Corresponding author. Email: [email protected] droplet radius Ri. The volume fraction fi is varied by two orders of

Lyu et al., Sci. Adv. 2019; 5 : eaav8081 3 May 2019 1 of 6


SCIENCE ADVANCES | RESEARCH ARTICLE

A M B Takeoff event C Explosion event


icr
op High-speed
ho
ne camera

view
Side

view
Side
Light
source

reflection
Substrate
Quartz lens Heated

Bottom
view
aluminum block
–4 ms 0 ms 3 ms 7 ms –0.6 ms –0.3 ms –0.2 ms 0 ms
Light
source 120 D E

80
High-speed
camera 40
–4 0 4 8 –0.6 –0.3 0

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Fig. 1. Experiments showing two different behaviors of evaporating ethanol droplets. (A) Experimental setup with two high-speed cameras mounted with long-
distance microscopes and a microphone for acquiring the sound signal. (B and C) Side views of a small (initial radius Ri ≈ 30 mm; radius in the leftmost image ≈ 17 mm)
and a large ethanol droplet (initial radius Ri = 1.9 mm; radius in the leftmost image ≈ 53 mm), respectively, in their Leidenfrost states. Scale bars, 100 mm. The tem-
peratures of the substrate are the same, Ts = 296°C. The small droplet in (B) remains levitated and eventually takes off; its levitation height versus time t − tt, where tt is
the takeoff time, is shown in (D). See also movie S1. The large droplet in (C) remains stably levitated on its vapor layer but finally explodes. The lower row in (C) (bottom-
view images) shows the top surface of the substrate at the levitating and exploding stages. A dark patch appears when the droplet is in contact with the substrate.
(E) Sound signal versus time t − te for the large droplet, where te is the time of explosion. An audible crack is heard at the time of explosion; see also movie S2 for a
recording of the large droplet with sound. Videos of different final fates of Leidenfrost drops are shown in the Supplementary Materials. a.u., arbitrary units.

magnitude, from 10−5 up to 10−3. Figure 2A shows the final stages of similarly as reported by Ma et al. (23). Furthermore, Bouillant et al.
evaporation of a suspension droplet with an intermediate initial vol- (24) recently noted that a single convective roll forms inside the drop-
ume fraction (fi = 10−4) and the substrate temperature (Ts = 296°C). let. On the basis of the typical time scale of the roll, the particles Stokes
The middle image corresponds to the time when the droplet is at its number St ~ 10−5 ≪ 1, and particles may thus be considered nearly
explosion radius Re. The droplet had shrunk from its much larger tracers (25). Hence, the simple rolling flow inside the droplet does not
initial radius Ri = 1.9 mm (not shown here). On the basis of the radius hinder particle accumulation at the interface. This rolling persists until
ratio, we estimate that the droplet is still 90% liquid at this stage. In the microparticles accumulate and form a static solid shell at the surface
immediate following frame, we see that the droplet has undergone a (24). In addition, Fig. 2C shows one of the pieces of debris remaining
violent explosion, which leads to a marked increase in its lateral size. after explosion of a droplet. We observed that these shells exist in the
We observed that all Leidenfrost droplets with initial size in the debris, similarly as evaporating colloidal droplets (19, 26). We expect
range of 1.1 to 2.5 mm and initial concentration in the range of 10−5 the concentration in the shell to approach the random close packing
to 10−3 end up exploding at their final stage. Thus, phenomeno- state (27), i.e., fs ≈ 0.64, while we expect that in the bulk of the drop to
logically, the final stages of evaporation of suspension droplets seem remain comparable to fs ~ 10−4. If the shell thickness scales with the
identical to those of large pure droplets. However, the explosion ra- droplet’s explosion radius, then mass conservation of the particles
dius Re varies for the different cases; while for a suspension droplet Re results in
can be as large as 0.5 mm, for the pure droplets we observe explosions
at Re ~ 50 mm. Re =Ri º fi
1=3
ð1Þ

DISCUSSION In Fig. 2D, we plot Re/Ri versus fi. The scaling holds remarkably
We develop a model to understand the influence of suspended par- well for the entire range of fi in our experiments. Further, Re /Ri is
ticles on the droplet explosion radius. For the droplet as shown in nearly independent of temperature and initial radius, as shown by
Fig. 2A with Ri = 1.9 mm, fi = 10−4, and Ts = 296°C, the typical du- the insets to Fig. 2D. Using the experimental values of Ri, fi, and Re,
ration of evaporation tdry ~ 20 s. The time scale of diffusion tmix ≈ we estimate the ratio of shell thickness to explosion radius s* ≈ 0.1 ±
R2/D > 103, where R is the radius of droplets and D is the diffusion 0.05. The measured shell thicknesses roughly agree with our expecta-
coefficient of particles in the liquid. The diffusion time scale tmix ≫ tion of particle accumulation.
tdry, implying that, as the evaporation proceeds, the particles would We further explore the physical mechanism that triggers the ex-
tend to accumulate and pile up at the droplet-air interface (see Fig. 2B). plosions (28). Sugiyama et al. (20) had anticipated that explosions
We also consider the effects of star-shaped oscillation and the inner of colloidal-polymer droplets might be triggered by local contact
flow of a droplet. When a droplet shrinks around or smaller than the with the substrate, whereas Moreau et al. (29, 30) postulated that for
capillary length scale, we do not observe any star-shaped oscillation, surfactant-laden droplets, a buildup of pressure within the droplet

Lyu et al., Sci. Adv. 2019; 5 : eaav8081 3 May 2019 2 of 6


SCIENCE ADVANCES | RESEARCH ARTICLE

Evaporating droplet Explosion While it has become clear that local contact occurs before the
A explosion, it remains to be explained what causes the stably levitated
Top view

drop (Fig. 3A, leftmost image) to suddenly touch down on the sub-
strate. Below, we model the vapor flow that levitates the evaporating
Leidenfrost droplet. When the size is much smaller than the capil-
lary length ℓc (ℓc ≈ 1.5 mm for ethanol), the droplet may be expected
to become nearly spherical. The bottom surface of the droplet is
–590 ms 0 ms 0.1 ms nearly flat (12, 31), with the horizontal extent (32) l ≈ R2/ℓc much
B C 100 smaller than the droplet radius (12, 13), and the temperature inside
Shell the droplet is nearly homogeneous (12, 24). For these droplets, the
evaporation rate can be expected to be nearly uniform at the inter-
Bulk face (12). Consequently, the volume flow rate of vapor per unit area
is given by

: rl dQ
D q¼ ð2Þ
4pR2 rv dt

where rv and rl are the vapor and liquid densities, respectively, and

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|dQ/dt| is the rate of volume change of the droplet, which can be
calculated from images of the evaporating droplet. Continuous evap-
oration between the droplet’s base and the substrate leads to an es-
caping thin layer of vapor, which exerts a high pressure on the drop.
Assuming that the vapor layer is in a quasi-steady state, the evaporation
flux of the flat region is equal to the radial flow flux in the vapor layer
(see Fig. 3B, inset), giving
:
“Pure” qr
vr ðrÞ ¼ ð3Þ
ethanol 2h

Here, vr(r) is the horizontal radial velocity in the vapor layer at a


distance r from the center of the flat region, and h is the thickness of
the vapor layer. Because the vapor layer thickness and its variation
Fig. 2. Explosion details of evaporating Leidenfrost droplets. (A) Top view of are very small as compared to its horizontal extent (12, 13, 31, 33),
an evaporating Leidenfrost droplet of ethanol with an initial contaminant volume h can be assumed to be independent of r (12, 31). In this limit, the lubri-
fraction fi = 10−4 and a substrate temperature Ts = 296°C. The middle image shows cation approximation can be used, which leads to a lift force (31)
the droplet at its explosion radius Re ≈ 150 mm, after having shrunk from an initial
vr r 2
F v ¼ 12pmv ∫o
radius Ri = 1.9 mm (not shown here; radius in the leftmost image ≈ 230 mm). The l
dr ð4Þ
rightmost image shows a violent explosion of the droplet, which leads to a marked h2
increase in its lateral size. (B) Schematic of particle accumulation at the receding
droplet interface during evaporation, leading to the formation of a shell. (C) Picture
where mv is the dynamic viscosity of the vapor. Under the condition of
of an experimental piece of explosion debris with a shell of accumulated particles.
Scale bar, 100 mm. (D) Ratio Re/Ri versus fi for exploding ethanol suspension droplets
stable levitation, the lift force balances the droplet’s weight containing
at various substrate temperatures and for different Ri. The solid line indicates fi
1=3 particles in suspension G = [rpQp + rl(Q − Qp)]g, where rp is the density
scaling. The top inset shows Re/Ri for a range of substrate temperatures at various of particles, Qp is the volume of particles, and g is the gravitational ac-
initial radii and fixed fi = 10−4. The bottom inset shows Re/Ri for a range of initial celeration. Integrating Eq. 4 and equating to G, we obtain an expression
droplet radii at various substrate temperatures and fixed fi = 10−4. Note that the for the evolving thickness of the vapor layer
black, red, blue, and magenta symbols correspond to substrate temperatures 204°,
231°, 296°, and 321°C, respectively, and the triangle symbols in (D) are predictions for  1=3
pure ethanol droplets based on the observed Re/Ri and by extrapolating the fi
1=3 3 mv rl R6 dQ
h≈ ð5Þ
scaling. The error bars represent the SD. 8 rv G ℓ4c dt

triggers explosion. For our suspension droplets, we look more closely Figure 3B shows the calculated vapor layer thickness h versus the
into the events leading up to the explosion (see Fig. 3A). In the first time to explosion t − te, where te is the explosion time. The liquid with
image, the droplet is in a stably levitated state, as revealed by the side particles can still evaporate, although the thickness of the vapor layer
and bottom views. In the second image at ~t ¼ 0:1 ms, the bottom decreases as time. When the particles have accumulated to such an
view indicates local contact with the substrate. This can trigger sudden extent that the liquid at the interface is not enough to fill around the
boiling at the contact point and lead to the explosion seen in the right- particles, the roughness length scale of the droplet interface becomes
most image. An almost identical local contact triggers the explosion for comparable to the particle size. As evident from Fig. 3B, when h
the other droplets studied, as well as for pure droplets (see Fig. 1C, approaches around this critical thickness, the droplet locally contacts
bottom row). the heated substrate, thereby triggering the explosion. The same

Lyu et al., Sci. Adv. 2019; 5 : eaav8081 3 May 2019 3 of 6


SCIENCE ADVANCES | RESEARCH ARTICLE

A B C

Fig. 3. Local contact and explosion modeling of evaporating Leidenfrost droplets. (A) Side and bottom views of a suspension droplet just before and at the point
of explosion; here, Ri = 1.6 mm, fi = 10−4, and Ts = 296°C. Scale bars, 200 mm. (B) Vapor layer thickness h versus time to explosion t − te for an evaporating drop, where h
was estimated using Eq. 5. We find that the explosion occurs when h approaches 1 mm, which is comparable to the particle size. The inset shows a schematic of the
levitation model used in the estimation of h. (C) Thickness he of the vapor layer (calculated) at explosion, for droplets with fi varying from 10−5 to 10−3. Note that he

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stays nearly constant (~1 mm), i.e., comparable to the particle size. (D) Surface averaged volume flow rate, q, when the vapor layer is 1 mm thick. Note that q decreases
 

with fi, suggesting that the accumulation of the particles at the droplet interface inhibits evaporation. The error bars represent the range of the data.

holds for other initial concentrations fi. Figure 3C shows that the sulting contact with the substrate, has not yet formed. Hence, the small
vapor layer thickness at explosion he is around 1 mm for all volume droplet rises up above the substrate and escapes its explosion fate.
fractions tested. At this stage, the evaporation may be limited by the Comparing the explosion radius Re and the takeoff radius Rt, we find
liquid flow through the porous shell formed on the droplet’s surface. that a large droplet (Re > Rt) first shrinks to the explosion radius, contacts
:
Because the shell formed is thicker for the larger fi cases, q decreases the substrate, and explodes, while a small droplet (Rt > Re) shrinks to the
with increasing fi (see Fig. 3D). takeoff radius and rises away from the substrate. While Re strongly de-
How can the explosion of suspension droplets be insightful to pure pends on the initial conditions of the droplet, we found that the takeoff
liquid droplets? First, the images of exploding pure liquid droplets are radius, Rt ≈ 14 to 16 mm, is only weakly affected by initial size and con-
similar to those of suspension droplets (see Figs. 1C and 3A). Further- tamination levels. Therefore, we can use Re = Rt as a criterion to calculate
more, for the pure droplets of various initial radii tested, we found that the critical (or transitional) initial radius, Ric, that separates the takeoff
the dimensionless explosion radius remains constant (Re/Ri ≈ 0.25 ± regime from the explosion regime. Figure 4B shows a prediction of Ric as
0.002). We extrapolate the scaling dependence between Re/Ri and fi to applied to pure and suspension droplets with varying levels of contam-
pure ethanol (see triangle symbols in Fig. 2D). This yields a prediction ination fi, at Ts ≈ 300°C. For a droplet of perfectly pure liquid (fi = 0),
of fi ≈ 2 × 10−6, which is a good estimate of the contamination levels in there should be no explosion, regardless of the droplet’s initial size, be-
analytical reagent of ethanol. cause Ric → ∞ for fi = 0. However, in practice for pure droplets with
Because Re/Ri is independent of the initial radius (Fig. 2D, bottom unavoidable contaminations (fi ~ 2 × 10−6), Ric ≈ 0.6 mm. With
inset), we can say that as the initial droplet size reduces, the explosion increasing contamination, Ric decreases, until it reaches about 100 mm
radius also becomes smaller. However, at some critical initial radius Ric, at fi = 10−3. In this situation, explosion becomes the likely fate of evap-
the droplet size R approaches the thickness of the vapor layer h. In this orating Leidenfrost droplets. Note that the Ric versus fi prediction in
limit, the lubrication model (in Eq. 4) will no longer be valid, and the Fig. 4B was obtained using the takeoff radius Rt = 15 ± 1 mm we observed
droplet then enters the takeoff regime (in this regime, the convective for pure and “suspension” droplets. Although the particles do not seem
heat flux is negligible compared to the diffusive flux) and spontaneous- to affect the value of Rt, their effect will become prominent at high par-
ly rises away (16, 17). In this regime, Celestini et al. (16) balanced the ticle concentrations. This deserves further studies in the future.
drag force and the weight of the droplet and derived a scaling law re-
lating the droplet’s elevation to its radius: h/R º R−3/2. We measured
the dimensionless elevation height h/R of ethanol droplets as a function CONCLUSION
of the radius R during the evaporation from the experiment using the In summary, we have shown that both initial size and level of con-
high-speed images (see Fig. 1B) and find a good agreement between tamination determine the fate of Leidenfrost droplets. Large droplets
our data and the −3/2 scaling law (see Fig. 4A). We define the maximal explode and small droplets take off at the final Leidenfrost stage. The
radius that satisfies this scaling relation as the takeoff radius Rt for pure dimensionless explosion radius has a 1/3 power-law dependence on
droplets and, similarly, for suspension droplets. After the droplet has the initial volume fraction of particles fi. The explosion is caused by
shrunk to Rt, it stays in a quasi-static state and steadily rises as the evap- contaminants, which accumulate at the interface as the droplet evap-
oration proceeds. We found that for pure and suspension droplets of orates and concurrently decrease the evaporation rate. When the
ethanol, Rt lies in the range 15 ± 1 mm, which is much larger than these vapor layer thickness approaches the contaminant microparticle
small droplets’ predicted explosion radii. Thus, an evaporating small radius, the droplet locally contacts the hot substrate and explodes.
droplet reaches the takeoff radius well before its explosion radius. At In this situation, the contaminant particles could act as a nucleus
this stage, the shell, which causes the reduced evaporation and the re- for the sudden boiling event. Furthermore, it is also plausible that

Lyu et al., Sci. Adv. 2019; 5 : eaav8081 3 May 2019 4 of 6


SCIENCE ADVANCES | RESEARCH ARTICLE

A help develop novel strategies for controlled particle transport and dep-
osition using the Leidenfrost effect. For instance, Leidenfrost droplets
Time could serve as carriers of microcomponents in electronics (6), wherein
their transport and deposition can be controlled by tuning droplet size
and particle concentration. Other avenues could lie in heat transfer
enhancement, wherein the addition of impurities can trigger the early
loss of Leidenfrost state. Last, the robust radius ratio versus particle
concentration scaling we uncovered here opens up the possibility of
developing new techniques to assess the purity of liquid samples.

MATERIALS AND METHODS


Experimental methods
The experiments had to be performed in a very clean environment.
The following procedure was adopted for cleaning the needle, quartz
substrate, and spray nozzle used in the experiments. Before each ex-
periment, the components were immersed in acetone and placed in
“Pure” Suspension droplets an ultrasonic bath for 2 min. The same procedure was repeated with

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ethanol and finally using ultrapure water. After this, purified com-
B pressed air was blown to dry the components. An air purifier in the
laboratory ensured a clean environment during the experiment.
The experiments were performed using a variety of liquids includ-
Explosion regime ing ultrapure water, ethanol, methanol, butanol, acetone, and hydro-
fluoroethers (Novec 7000 and Novec 7100 from 3M Ltd.). The droplets
0.6 mm
were deposited on a slightly curved quartz substrate. The top surface of
the substrate has a curvature radius of 114.5 mm, allowing us to keep
droplets in the camera field of view (see Fig. 1A). The substrate was
placed on a heated aluminum block controlled by a PID (proportional,
integral, derivative) controller. The surface temperature Ts of the sub-
Takeoff regime strate was measured with a thermocouple that was stuck to the sub-
strate. Two sets of high-speed cameras with long-distance microscopes
were used to record the evaporation process from the side and below
simultaneously. The side-view recordings were used to measure the ra-
dius, elevation, and state of droplets, while the bottom-view images
served to distinguish levitation from contact with the substrate. When
Fig. 4. Predictions of takeoff and explosion regimes for pure and suspension a vapor layer exists, the strong reflected light results in a bright spot
droplets of ethanol. (A) Dimensionless elevation h/R of a small pure ethanol drop- around the base of the droplet. When the droplet contacts the substrate,
let as a function of its radius R, as measured from experiment by using the high-
the wetted area is seen as a dark patch (15, 33, 34).
speed images, at Ts = 296°C. At a takeoff radius Rt ≈ 15 mm (vertical dashed line), the
shrinking droplet enters a quasi-static regime and follows the scaling h/R º R− 3/2.
A spray generator was used to produce small ethanol droplets. The
(B) Predicted critical initial radius Ric versus contamination level fi for Ts = 296°C. initial size of droplets Ri was in the range of 19 to 52 mm, and the av-
This Ric separates the explosion regime from the takeoff regime. For pure ethanol erage size was about 30 mm. A board with an opening was placed be-
drop (fi ≈ 2 × 10−6), Ric ≈ 0.6 mm. With increasing contamination fi, Ric decreases, tween the spray and the substrate to reduce the number of droplets
which makes explosion the more likely outcome. falling in the observation area. Larger droplets with Ri larger than
0.9 mm were created using a microliter pipette. Figure 1 (B and C)
compares the Leidenfrost dynamics of two droplets of very different
the local contact is aided by the gravitational settling of clumped initial radii.
TiO2 particles; however, this deserves further study in future. We
observed the same two final fates for a variety of pure liquids (lab- Preparation of the suspension
oratory grade; nonvolatile residue, ~1 ppm), including ultrapure The amount of hydrophilic rutile titanium dioxide (TiO2) micropar-
water, ethanol, methanol, butanol, acetone, and hydrofluoroethers ticles (from Macklin) to be added was weighed using an electronic bal-
(Novec 7000 and Novec 7100). Therefore, one can conclude that ance. For particles, the radius Rp is about 1 mm and the purity is about
the two regimes witnessed here are general to the fate of evaporating 99%. Controlled quantities were added to laboratory-grade ethanol for
Leidenfrost droplets—the initial size of droplet has a major influence obtaining different particle concentrations. Ethanol was chosen for the
on its final fate. experiments because its low surface tension limits the amount of con-
The present research has also solved the mystery of the audible taminants within the droplets and its low latent heat enables a high
crack heard by Leidenfrost (1) in 1756 and, at the same time, provided evaporation rate. The different concentrations of suspensions were
a unified understanding of the final stage of Leidenfrost dynamics ap- stored in airtight bottles. To avoid the deposition of the microparticles,
plicable to pure and suspension droplets, bridging nearly three orders before each sampling, the bottles were immersed in the ultrasonic bath,
of magnitude variation in initial concentration. These insights could and then the suspension was shaken vigorously with a vortex shaker

Lyu et al., Sci. Adv. 2019; 5 : eaav8081 3 May 2019 5 of 6


SCIENCE ADVANCES | RESEARCH ARTICLE

from Kylin-Bell (product number: VORTEX-5). To further avoid the 16. F. Celestini, T. Frisch, Y. Pomeau, Take off of small Leidenfrost droplets. Phys. Rev. Lett.
109, 034501 (2012).
possibility of particles segregating, the syringe used for the experiment
17. D. V. Zaitsev, D. P. Kirichenko, V. S. Ajaev, O. A. Kabov, Levitation and self-organization of
was also shaken before each experiment. liquid microdroplets over dry heated substrates. Phys. Rev. Lett. 119, 094503 (2017).
18. E. Oberdörster, Manufactured nanomaterials (fullerenes, C60) induce oxidative stress
Image processing in the brain of juvenile largemouth bass. Environ. Health Perspect. 112, 1058–1062
The boundary of the droplet was identified using MATLAB, and a (2004).
19. N. Tsapis, E. R. Dufresne, S. S. Sinha, C. S. Riera, J. W. Hutchinson, L. Mahadevan,
circle fitting function (35) was used to obtain the radius of the droplet D. A. Weitz, Onset of buckling in drying droplets of colloidal suspensions. Phys. Rev. Lett.
R and the position of the center of the droplet. For the explosion re- 94, 018302 (2005).
gime, the droplet radius R was used to estimate the volume of the 20. Y. Sugiyama, R. J. Larsen, J.-W. Kim, D. A. Weitz, Buckling and crumpling of drying droplets
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Lyu et al., Sci. Adv. 2019; 5 : eaav8081 3 May 2019 6 of 6


Final fate of a Leidenfrost droplet: Explosion or takeoff
Sijia Lyu, Varghese Mathai, Yujie Wang, Benjamin Sobac, Pierre Colinet, Detlef Lohse and Chao Sun

Sci Adv 5 (5), eaav8081.


DOI: 10.1126/sciadv.aav8081

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