Soil Science and Plant Nutrition

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Drop size dependence of soil-water contact angle

in relation to the droplet geometry and line
tension

Dewpura A. L. Leelamanie & Jutaro Karube

To cite this article: Dewpura A. L. Leelamanie & Jutaro Karube (2012) Drop size dependence of
soil-water contact angle in relation to the droplet geometry and line tension, Soil Science and Plant
Nutrition, 58:6, 675-683, DOI: 10.1080/00380768.2012.745798

To link to this article: https://doi.org/10.1080/00380768.2012.745798

Published online: 13 Dec 2012.

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Soil Science and Plant Nutrition (2012), 58, 675—683 http://dx.doi.org/10.1080/00380768.2012.745798

ORIGINAL ARTICLE

Drop size dependence of soil-water contact angle in relation to the

droplet geometry and line tension
Dewpura A. L. LEELAMANIE1,2 and Jutaro KARUBE2
1
Faculty of Agriculture, University of Ruhuna, Mapalana, Kamburupitiya, Sri Lanka and 2Faculty of Agriculture, Ibaraki
University, 3-21-1 Chuo, Ami-machi, Ibaraki-ken, Japan

Abstract
The soil-water contact angle is used as a measure of the surface hydrophobicity of soils. The contact angle for
particular solid—liquid combination is considered to vary with the drop size. In this paper, we focused on
examining the drop size dependence of contact angle on soil surfaces compared with homogeneous solid
surfaces, and determining its relation to the droplet geometry and line tension. The contact angle estimated
using geometric parameters of the droplets (G) showed decreasing trend with increasing drop size from 5 to
50 mL irrespective of the deformations in the droplet shape in larger drops. This was considered to be a result
of the corresponding deviations of the geometric parameters of the droplets. The directly measured contact
angle (A) first decreased and then increased with increasing drop size from 5 to 50 mL. The drop size at lowest
A for hydrophobized silica sand with 1 g kg—1 stearic acid (SA) and the acryl surfaces was 20 mL, whereas that
for hydrophobized silica sand with 5 g kg—1 SA and siliconed paper was 30 mL. The decrease in A with
increasing drop size was explained as a result of the line tension effect using the modified Young’s equation.
Despite the surface heterogeneity, all the surfaces tested in this study showed positive line tensions on the
order of 10 mJ m—1. Irrespective of the heterogeneity of the surfaces, the A in this experiment agreed with the
modified Young’s equation for drop sizes up to about 20—30 mL, where the A and G were also in good
agreement. Drop size dependence of contact angle was independent of the level of surface hydrophobicity.
The A on all the examined surfaces started to increase with increasing drop size when the deformation index,
Id, exceeded 5%, where the wetting radius, R exceeded the capillary length. The increase in A with increasing
drop size was attributed to the deformations of water drops due to the effect of gravity.
Key words: contact angle, drop size, droplet geometry, hydrophobicity, line tension.

INTRODUCTION The soil-water contact angle is used as a measure of

Droplet shape and the dynamics of its spreading play an
important role in nature and many areas of science and
technology. The contact angle is a measure of the ability
of a liquid to spread out on a solid surface, showing the
resultant between cohesive and adhesive forces between
solid and liquid.
Correspondence: D.A.L. Leelamanie, Faculty of Agriculture,
Ibaraki University, 3-21-1 Chuo, Ami-machi, Ibaraki-ken 300-
0393, Japan. Tel: 029-888-8598. Fax: 029-888-8598. Email:
leelamanie@soil.ruh.ac.lk
Received 20 July 2012.
Accepted for publication 30 October 2012.
surface hydrophobicity of the soil where the magnitude
of contact angle varies depending on how wettable or
water repellent the surface is. The higher the contact
angle is, the more hydrophobic the soil surface becomes.
The main hydrological consequences of surface hydro-
phobicity, or the soil water repellency, are reduced
infiltration, increased overland flow, spatially localized
infiltration, or fingered flow development, etc. (Wallis
and Horne 1992; Kobayashi et al. 1996; Annaka and
Hanayama 2010). The contact angle is therefore of
practical importance in understanding the hydrologic
functions of unsaturated soils during natural wetting and
drying processes.
Of all the methods employed to measure the contact
angle, direct measurement from sessile drops is probably

ß 2012 Japanese Society of Soil Science and Plant Nutrition

676 D. A. L. Leelamanie and J. Karube
the most popular approach. The contact angle measure-
ments are easy to perform on smooth and flat surfaces.
When it comes to a granular material such as soil,
assessing surface properties such as contact angle is
considerably difficult due to the nature of soil surfaces.
The modified sessile drop method (SDM), which consists
of measuring the contact angle by placing a water drop
on a monolayer of soil, made it possible to perform
direct measurement of the contact angle on soil
(Bachmann et al. 2000).
The physical phenomena that are related to the shape
of liquid droplets on solid surfaces and solid-water
contact angles still face many challenging questions such
as the existence of multiple values of the contact angle for
a given solid—liquid—gas system (Li 1996). First, the
contact angle hysteresis that can be observed with
advancing and receding contact angles; second, the
time dependence of the contact angle (Leelamanie and
Karube 2009), and third, the drop size dependence of the
contact angle.
It is normally accepted that the contact angle for a
particular solid—liquid combination varies with the drop
size. Over the years numerous researchers (Herzberg and
Marin 1970; Good and Koo 1979; Gaydos and
Neumann 1987; Duncan et al. 1995; Drelich et al.
1996a, b; Amirfazli et al. 1998a, b, 2000; Gu 2001;
Rodrı́guez-Valverde et al. 2002; Letellier et al. 2007;
Gajewski 2008; Viswanadam and Chase 2012) have
studied and attempted to explain the fundamental
relationship between drop size and solid—liquid contact
angle. The majority of them reported that the contact
angle decreases with increasing drop size (Gaydos and
Neumann 1987; Amirfazli et al. 1998a, 2000; Gu 2001;
Vafaei and Podowski 2005), whereas some reported the
opposite (Good and Koo 1979; Viswanadam and Chase
2012) or no relation (Good and Koo 1979; Drelich et al.
1996a). These findings demonstrate that different results
for drop size dependence of contact angle can be
expected with different liquids and solids. For example,
Good and Koo (1979) reported that the water-teflon
contact angle decreased by about 8 , whereas n-decane-
teflon contact angle did not change, with decreasing drop
diameter from 4 to 1 mm (33 to 0.5 mL). However, most
of these findings, which were based on advancing and
receding contact angles, are difficult to relate to the
initial contact angle of sessile drops considered in the
present study.
In general, the variation of contact angle with drop size
is mostly explained in terms of the line tension (Adamson
1990; Li 1996; Amirfazli et al. 1998a, b; Gu 2001), or
the tension of the three-phase contact line. The line
tension is considered in analogy to surface tension, and
can be defined as the specific free energy, or the free
energy per unit length, of the three-phase contact line.
Alternatively, it can be defined mechanically as a force
operating in the three-phase line or as an extra tensile
force acting on this line. The well-known Young’s
equation connects contact angle with surface tensions
of the solid—gas, liquid—gas, and solid—liquid consider-
ing the equilibrium of the three-phase contact line for a
given solid—liquid—gas system. As the line tension is an
extra force operating in the three-phase contact line it
should also be included in the equilibrium of this line.
Besides the effect of line tension, another explanation
for the drop size dependence contact angle is the effect of
surface heterogeneity (Drelich et al. 1996a; Rodrı́guez-
Valverde et al. 2002). Rodrı́guez-Valverde et al. (2002)
explained that if the volume of a drop placed on rough
surfaces increases, the three-phase contact line stands still
with the height of the drop increasing until the drop
relaxes and obtain a new contact line with greater radius.
They further explained that roughness increases the
contact angle if the angle is greater than 90 , but
decreases the angle if it is less than 90 .
Almost all the reported findings in the literature on the
contact angle as a function of drop size are measured on
smooth, planar, and homogeneous solid surfaces such as
teflon (Good and Koo 1979; Gaydos and Neumann
1987; David et al. 2009), metal (Gajewski 2008), fluoro
compound coated mica (Duncan et al. 1995), and
hydrophobic FC725 coated glass surfaces (Gu 2001).
Some researchers studied the drop size effect on biolog-
ical surfaces such as dentin (Wege et al. 2002) and wood
(Rodrı́guez-Valverde et al. 2002), or on artificially
induced periodically heterogeneous solid surfaces such
as grooved surfaces (J. Yang et al. 2009), and different
kinds of patterned surfaces (Drelich et al. 1996a;
Brandon et al. 2003). It is of prime importance to
understand how the contact angle of water over the soil
surfaces varies with drop size, and how it differs from the
drop size dependence of contact angle on homogeneous
and heterogeneous solid surfaces reported in the litera-
ture. In this study, we focused on examining the drop size
dependence of contact angle on model soil surfaces, as
measured by SDM, compared with homogeneous solid
surfaces, and on determining its relation to the droplet
geometry and line tension.
MATERIALS AND METHODS
Experimental setup
Two smooth, planar, homogeneous surfaces and two
rough comparatively heterogeneous model soil surfaces
with different hydrophobicities were used for the contact
angle measurement. Although all the surfaces that can be
prepared in the laboratory would have some degree of
heterogeneity for many reasons (Lin and Li 1995);
 D.A.L. Leelamanie and J. Karube 677

Table 1 Particle size distribution of silica

sand used in the experiment

Particle size (mm) Mass (%)

250—106 52.4
106—53 42.1
53—38 3.2
38—20 1.0
20> 1.3

siliconed poly-laminated papers adhered to glass slides

and acryl disks were used as comparatively smooth,
planar, and homogeneous surfaces. Rough heteroge-
neous model soil surfaces were prepared using silica sand
(Tohoku Keisha Co., Yamagata, Japan) hydrophobized
with stearic acid (SA) (molecular weight 284.5, Wako
pure chemical industries, Osaka, Japan) to obtain 1 and
5 g kg—1 contents. The particle size distribution of silica
sand is given in Table 1. Hydrophobized silica sand was
fixed on a double-sided 1.5 cm  1.5 cm adhesive tape
pasted on a glass slide (Leelamanie et al. 2008a). The
experiment was conducted in a constant temperature
room, with 25 C and 75  5% relative humidity. All the Figure 1 Geometric parameters for calculating contact angle
(G) when (a) G < 90 and (b) G > 90 . O, geometric origin; h,
prepared samples were kept in a sealed chamber under actual droplet height; r, radius; x, wetting radius of the droplet;
75% relative humidity, maintained using saturated G, contact angle estimated using geometric parameters of the
sodium chloride (NaCl) solution (Leelamanie et al. droplet.
2008b), for 48 h before the contact angle measurement.
For  4 90:
ð2Þ
Contact angle measurement G ¼  þ 90
The contact angle on each surface was measured using
the SDM (Bachmann et al. 2000). Using two adjustable sin  ¼ ðh  rÞ=r ð3Þ
micro-pipettes (PipetGene, TGK, Tokyo, Japan), differ-
ent sizes of deionized water drops (5, 10, 15, 20, 30, 40, Deformation index
and 50 mL, 1% accuracy) were placed separately on the
In a situation where the droplet is in perfect spherical cap
prepared surfaces in six replicates per surface, per drop
shape and no deformation has occurred, the ratio
size, and digital microphotographs of the horizontal view
between vertical (RV) and horizontal (RH) radii is
of the deionized water drops were taken within 1 s using
equivalent to one. With increasing drop size the drop
a digital microscopic camera (Leelamanie et al. 2008a).
shape is thought to be affected by the force of gravity
Using the microphotographs, the contact angle of each
(Whyman and Bormashenko 2009), or the drop weight,
sample was directly measured using a protractor (A)
and the vertical radius might deviate from the geometric
considering the average of the contact angles of the drop
radius to obtain a lower value than that expected in the
at both three-phase contact points. The contact angle
case of a perfect spherical droplet. Considering a basic
was estimated as described in Equations 1—3, and Fig. 1,
situation where the water drop would make a perfect
using the geometric parameters of the droplet (G) as they
spherical cap on the solid surface (no deformation in the
appeared in the same microphotographs that were used
shape of the droplet), the percentage asymmetrical
to obtain A considering a spherical approximation
deviation, or the deformation index Id, was obtained
(M.W. Yang and Lin 2003; Annaka 2006; Stalder
using the following equation:
et al. 2010):
Id ¼ ð1  RV =RH Þ  100 ð4Þ
For  5 90:
ð1Þ In the case of highly hydrophobic surfaces where the
G ¼ 2 tan1 ðh=xÞ
contact angles are larger than 90 , the RV and RH can be
678 D. A. L. Leelamanie and J. Karube
Figure 2 Illustration showing the geometric parameters for the
calculation of horizontal and vertical radius of the drop for
contact angles smaller than 90 . A, directly measured contact
angle; RH, horizontal radius; h, actual droplet height; a,
difference between geometric radius and actual droplet height;
x, wetting radius of the droplet.
easily measured as they are observed on the micropho-
tograph of the water droplet. In contrast, on surfaces
with lower hydrophobicities with contact angles below
90 , the RV and RH are not easily observed on the
microphotographs. For that situation, RV and RH were
estimated combining the geometric parameters of the
droplet with the actual droplet height (h) as explained in
Equations 5—7 and Fig. 2:
RV ¼ h þ a ð5Þ
x contact angle. Considering the surface heterogeneity,
a¼ ð6Þ
tan A
x contact angles below 90 and above 90 . Our results,
RH ¼ ð7Þ
sin A
RESULTS AND DISCUSSION
The effect of drop size on sessile drop contact angle of
hydrophobized silica sand with 1 and 5 g kg—1 SA
contents, siliconed paper, and acryl are respectively
shown in Fig. 3a, b, c, and d.
The contact angle estimated using geometric parame-
ters of the droplet (G) showed a decreasing trend with
increasing drop size. The G of silica sand with
1 g kg—1 SA, 5 g kg—1 SA, siliconed paper, and acryl sur-
faces decreased from 98 to 86 , 112 to 101 , 106 to
88 , and 72 to 62 , respectively, with increasing drop
size from 5 to 50 mL.
As explained in Fig. 1, Equations 1—3 for contact angle
calculation have been developed assuming a perfect
spherical cap shape for the water droplet. This
assumption can be justified for smaller drop sizes. With
increasing drop size, the spherical shape gradually
deforms to become oblate spheroidal in shape
(Whyman and Bormashenko 2009), showing lower
droplet height, (h in Fig. 1) than the expected.
Accordingly, the deformation of the droplet shape
would always result in a decrease in G with increasing
drop size as explained in Equations 1—3, irrespective of
the corresponding changes in the apparent contact angle.
In contrast to the G, the directly measured contact
angle (A) of all the tested surfaces first decreased and
then increased with increasing drop size from 5 to 50 mL.
For silica sand hydrophobized with 1 g kg—1 SA, the A
first decreased from 96 to 92 with increase in water
drop size from 5 to 20 mL, and thereafter very slightly
increased up to 50 mL drop size. The A on the surface of
silica sand hydrophobized with 5 g kg—1 SA first
decreased from 112 to 102 with increase in water
drop size from 5 to 30 mL but increased up to 105 with
increasing drop size from 30 to 50 mL. The A obtained
on the siliconed paper decreased from 102 to 92 with
increase in drop size from 5 to 30 mL, and increased to
reach 96 at 50 mL drop size. The A for acryl first
decreased from 73 to 64 with increase in water drop
size from 5 to 20 mL and thereafter increased up to 75 at
50 mL drop size. The A and G are in good agreement for
all the tested surfaces until A started to increase with
increasing drop size.
The results obtained in this study for smooth homo-
geneous and rough heterogeneous surfaces showed a
comparable pattern in the drop size dependence of
Rodrı́guez-Valverde et al. (2002) explained that drop size
dependence of contact angle is different for surfaces with
however, showed that the drop size dependence of
contact angle is independent of the level of surface
hydrophobicity in both homogeneous and heterogeneous
surface conditions.
The result shows two different phases for the
variation of the A with the drop size. The first
phase, or the decrease of the contact angle with
increase in drop size, might be explained using the
line tension phenomenon.
Contact angle describes the edge of the two-phase
boundary (e.g., solid-water) where it ends at a third
phase (e.g., gas). The contact angle and the surface free
energies of solid—gas, liquid—gas, and solid—liquid
interfaces are related in the well-known Young’s equa-
tion (Young 1805), considering the force balance of a
situation where a liquid drop is placed on a smooth solid
surface and allowed to come to equilibrium.
Young stated that when a liquid makes contact with a
solid surface it will approach the contact line following a
 D.A.L. Leelamanie and J. Karube 679

Figure 3 Effect of drop size on sessile drop contact angle of (a) hydrophobized silica sand with 1 g kg—1 stearic acid (SA), (b)
5 g kg—1 SA, (c) siliconed paper, and (d) acryl. A, directly measured contact angle; G, contact angle estimated using geometric
parameters of the droplet. Error bars indicate  standard deviation.

dihedral angle, , which depends on the solid—gas,
liquid—gas, and solid—liquid interfacial tensions. For
the equilibrium of the water drop, the force balance of
the horizontal direction can be given by:
lg cos  ¼ sg  sl ð8Þ
where  is the contact angle (equivalent to A in the
present study), and gsg, glg, and gsl are the solid—gas,
liquid—gas, and solid—liquid interfacial tensions. Young’s
equation primarily implies that for given interfacial
tensions the contact angle is drop size-independent
(Vafaei and Podowski 2005 and references therein).
Young’s equation is derived only for the simplest, ideal
systems, and associated with several very restrictive
conditions. The equation has been developed without
considering many important factors that would affect the
force balance of the system at equilibrium, such as the
effects of the three-phase contact line. The line tension is
considered as an extra tensile force acting on the three-
phase line.
Therefore, for the equilibrium of the water drop, line
tension should be included in the force balance of the
horizontal direction, and the modified Young’s equation
can be expressed as:
lg cos  ¼ sg  sl  =R ð9Þ
where  denotes the line tension of the three-phase
contact line and R denotes the radius of the three-phase
contact circle (Li 1996).
Equation 9 clearly states that the contact angle
decreases with the increase in the wetting radius, or the
drop size. Although this equation would be satisfactory
for truly axisymmetric drops on planar, homogeneous
solid surfaces with a smooth three-phase contact circle,
the A in this experiment agreed with the equation up to
680 D. A. L. Leelamanie and J. Karube

Figure 4 Deformation index (Id) and the radius of the three-phase contact surface, or the wetting radius (R), against the drop size for
(a) hydrophobized silica sand with 1 g kg—1 stearic acid (SA), (b) 5 g kg—1 SA, (c) siliconed paper, and (d) acryl.

about 20—30 mL drop size irrespective of the roughness
or the smoothness of the tested surfaces.
As the modified Young’s equation is applicable for an
axisymmetric drop on an ideal solid surface, it is under
the assumption that the contact angle is not sensitive to
the drop’s weight, and the effect of gravity on the drop
shape would be negligible. If the liquid drops used in
contact angle studies are of small volume, the contribu-
tion of the effect of gravity to the contact angle may often
be neglected in comparison to the surface tension effects.
However, this is not applicable for larger drops.
Interactions between gravity and adhesive forces play
an important role in a variety of wetting phenomena, and
can be described using capillary length (l):
rffiffiffiffiffiffi
lg
l¼
g
where  is the density of the liquid and g is the
acceleration due to gravity (Whyman and Bormashenko
2009). When the drop size is much smaller than l, the
spherical model for droplet on a solid surface is still
relevant and the effect of gravity may be neglected.
However, when the drop size reaches the capillary length
(2.71 mm for water at 25 C) the drop shape would be
affected by gravity and the spherical model will no longer
be accurate.
Considering that the drop shape is not spherical for
larger drops, the deformation index (Id) and the radius of
the three-phase contact surface, or the wetting radius (R),
were graphed against the drop size, and shown in Fig. 4.
The Id started to increase with increasing drop size for
drops larger than 10—15mL. According to Figs. 3 and 4,
A decreased with increasing drop size when the Id
remained below 5%. The A started to increase with
increasing drop size when the Id exceeds 5%, where the
wetting radius, R exceeds the capillary length (2.7 mm),
except in the case of acryl where the increase of A started
when R exceeds 2.9 mm. Considering these results, the
ð10Þ
increase in A with increasing drop size was attributed to
the deformation of water drops due to the effect of
gravity. In contrast to Benselama et al. (2011) who
reported that the effect of gravity becomes more
pronounced at contact angles around 90 , the gravity
effect showed no relation to the level of hydrophobicity
of the tested surfaces.

Figure 5 The correlation between cos  and 1/R for (a) hydrophobized silica sand with 1 g kg—1 stearic acid (SA), (b) 5 g kg—1 SA,
(c) siliconed paper, and (d) acryl. A, directly measured contact angle; R, wetting radius; x, horizontal figure axis; y, vertical figure axis.
When the radius of the three-phase contact circle, R,
reaches infinity in the case of infinitely large drops, /R
will be zero and Equation 9 will be replaced by the
classical Young’s equation (Eq. 8).
For the equilibrium of the three-phase contact line
corresponding to an infinitely large drop, Equation 9 can
be rewritten as:
lg cos 1 ¼ sg  sl
where 1 is the contact angle corresponding to an
infinitely large drop (R ¼ 1). Provided that line tension,
liquid surface tension, and cos 1 are constants for a
given solid—liquid system, combining Equations 80 and 9,
a linear correlation can be stipulated between cos  and
1/R (Li 1996):
 1
cos  ¼ cos 1 
lg R
D.A.L. Leelamanie and J. Karube 681
The  and the 1 can be determined from the slope
(/glg) and the intercept (cos 1) of the specified line.
As it was clear from the results that the drop shape and
the A were considerably affected by gravity for water
drops larger than 20 mL for hydrophobized silica sand
with 1 g kg—1 SA and acryl surfaces, and 30 mL for
hydrophobized silica sand with 5 g kg—1 SA and siliconed
paper surfaces, linear correlation between cos A and 1/R
ð80 Þ was developed for each surface only up to those critical
drop sizes (Fig. 5). The  for each surface was determined
from the slopes of the lines.
There is no consistency in the reported literature for
the sign and the order of magnitude of the line tension.
To satisfy a stable thermodynamic equilibrium, the line
tension should be positive for an ideal solid—liquid
system (Li 1996). However, there is much scientific
evidence available for positive (Amirfazli et al. 1998a, b,
2000; Gu 2001; J. Yang et al. 2009) and negative
ð11Þ
(Drelich et al. 1996b; J. Yang et al. 2009) signs of the line
682 D. A. L. Leelamanie and J. Karube
tension. Since liquid surface tension glg is always positive,
a negative slope indicates a positive line tension, and a
positive slope indicates a negative line tension. According
to Equation 9, as the radius of the three-phase contact
line R increases, contact angle will decrease if the line
tension is positive, or increase if the line tension is
negative. According to Fig. 5, all the surfaces used in this
study showed negative slopes, corresponding to positive
line tensions. Line tensions for hydrophobized silica sand
with 1 and 5g kg—1 SA contents, siliconed paper, and
acryl, were 24, 36, 44, and 50 mJ m—1, respectively.
The magnitude of the line tensions is mostly reported to
vary from the order of 1 (Duncan et al. 1995; Gaydos and
Neumann 1987; Gu 2001) to 100 (Amirfazli et al.
1998a) mJ m—1. Our findings lie between these values
showing a magnitude of line tensions on the order of
10 mJ m—1.
Conclusions
The contact angle estimated using geometric parameters
of the droplet (G) showed a decreasing trend with
increasing drop size from 5 to 50 mL irrespective of the
deformations in droplet shape in larger drops. This was
considered a result of the corresponding deviations of the
geometric parameters of the deformed droplets. In
contrast to the G, the directly measured contact angle
(A) first decreased and then increased with increasing
drop size from 5 to 50 mL. Irrespective of the heteroge-
neity of the surfaces, the A on all the tested surfaces in
this experiment agreed with the modified Young’s
equation up to about 20—30 mL drop size, where the A
and G were also in good agreement. The drop size
dependence of contact angle is independent of the level of
surface hydrophobicity. The decrease in the contact angle
with increasing drop size was explained using the line
tension phenomenon. All the surfaces tested in this study
showed positive line tensions on the order of 10 mJ m—1.
No evidence was found for the differences in drop size
dependence of contact angle between rough, heteroge-
neous, soil surfaces and smooth, homogeneous surfaces.
The Id started to increase with increasing drop size for
drops larger than 10—15 mL. The A on all examined
surfaces started to increase with increasing drop size
when the Id exceeds 5%, where the wetting radius R
exceeds the capillary length. The increase in A with
increasing drop size was attributed to the deformation of
water drops due to the effect of gravity.
To obtain comparable contact angle measurements for
different soils, the drop size can be considered a function
of prime importance. Drop size of <15 mL can be
recommended for soil-water contact angle measurements
to avoid superfluous effects caused by deformations in
drop shapes.
ACKNOWLEDGMENTS
The Japan Society for the Promotion of Science is
gratefully acknowledged for providing an Invitation
Fellowship for Research in Japan (Long-Term).
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