Eaav8081 Full
Eaav8081 Full
INTRODUCTION RESULTS
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
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
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
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
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
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
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.
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
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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
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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
sphere droplet Q ¼ 43 pR3 . Then, we used Eq. 5 to calculate the thick- of colloid-polymer suspensions. Langmuir 22, 6024–6030 (2006).
21. M. Osękowska, E. Karuga-Kuźniewska, D. Wojcieszak, M. Mazur, A. Poniedzialek,
ness of the vapor layer. When the radius of the droplet suddenly in-
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creases sharply, it indicates that the droplet has exploded, and Re was surface properties of TiO2 thin films on the viability of L929 cells. Pol. J. Chem. Technol. 17,
defined as the radius just before explosion. For the large droplets created 33–39 (2015).
by the microliter pipette, we used a set volume to calculate the initial 22. K. He, F. Yang, Y. Ma, Q. Zhang, X. Yao, C. K. Chan, S. Cadle, T. Chan, P. Mulawa, The
radius of the droplet Ri. characteristics of PM2.5 in Beijing, China. Atmos. Environ. 35, 4959–4970 (2001).
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