Capillary filling dynamics of water in nanopores

Chirodeep Bakli and Suman Chakraborty

Citation: Appl. Phys. Lett. 101, 153112 (2012); doi: 10.1063/1.4758683

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 APPLIED PHYSICS LETTERS 101, 153112 (2012)

Capillary filling dynamics of water in nanopores

Chirodeep Bakli and Suman Chakrabortya)
Department of Mechanical Engineering, Indian Institute of Technology Kharagpur, Kharagpur 721302, India
(Received 9 July 2012; accepted 27 September 2012; published online 10 October 2012)
We portray a universal description of dynamic slip-stick behavior of water flowing through
nanoscale pores. Based on fundamental molecular transport considerations, we derive a generalized
constitutive model for describing resistive forces acting on the water column in a capillary that is
being dynamically filled, as a combined function of the meniscus height, surface wettability, and
roughness. This effectively acts like a unique signature of nanopore imbibition characteristics of
water, which, when substituted in a simple one-dimensional force balance model agrees
quantitatively with results from molecular dynamics simulations for a general class of problems,
without necessitating the employment of any artificially tunable fitting parameters. V C 2012

American Institute of Physics. [http://dx.doi.org/10.1063/1.4758683]

Fluid flows over nanometer length scales are faceted
with intriguing scientific and technological implications,
encompassing interdisciplinary applications ranging from
nanofluidic devices, porous nanomaterials, geophysics, to bio-
membranes,1,2 to name a few. With unprecedented advance-
ments in nanotechnology, the spontaneous ability of fluids in
penetrating through nanoscales pores3,4 has recently opened
up emerging possibilities of generating virtually one dimen-
sional nanostructures5,6 with multifarious functionalities.
Such devices and systems are often characterized with non-
trivial physical phenomena over molecular scales, involving
an intricate interplay between surface roughness, wettability,
and the capillary pressure gradient, in a spatio-temporally
evolving manner.
From a classical perspective, capillary filling dynamics
over system length scales is often represented by an elusively
simple yet richly insightful equation known as the Lucas-
Washburn (LW) equation,7,8 which essentially realizes a
dynamical balance of viscous and surface tension forces.
Taking the possibilities of interfacial  slip4lsinto
 account, this
equation assumes the form: 8pgL dL dt 1  R ¼ 2pcRcos h; g
being the fluid viscosity, c being the liquid-vapor surface ten-
sion coefficient, L being the capillary imbibition length at
time t, R being the capillary radius, and ls being the slip
length. Notably, in the literature,8,9 the parameter ls in the
context of capillary imbibition has been traditionally treated
as an adjustable parameter that may best be “trained” by fit-
ting the problem-specific molecular simulation data to mimic
itself, notwithstanding its fundamental genesis. The abstrac-
tion of molecular level phenomenon and associated devia-
tions from the macroscopically predicted behavior from the
above equation has been addressed using several considera-
tions such as multilayer sticking,10 entrance effects,11 modi-
fied hydrodynamic capillary radius,12 dynamic contact angle
(DCA), and inertia.13–15 As a consequence, the validity of
LW model over sub-continuum regimes has not remained far
from being controversial.
Here, we show that by obtaining a molecular-simula-
tion-synthesized closure model in terms of a dynamic slip
a)
Author to whom correspondence should be addressed. Electronic mail:
suman@mech.iitkgp.ernet.in.
length (DSL) that is sensitive to the surface roughness-
wettability coupling over molecular scales, capillary dynam-
ics of water in nanopores may be represented faithfully by
LW behavior. In sharp contrast to the reported literature, we
do not presume ls to be an adjustable parameter, but we
obtain it as a parameter sensitive to the molecular level cou-
pling between interfacial phenomena and bulk transport, in a
dynamic environment. Unlike the situation with classical
pressure-driven flows, our analysis takes into consideration
the fact that the pressure gradient acting across the liquid
column in a capillary being continuously filled evolves
dynamically, imparting a spatio-temporal variation in the re-
sultant DSL characteristics. Our derivations, thus, essentially
do recognize the fact that the ls for a given contact angle and
roughness characteristic is a function of the driving force
(realized in the form of a dynamically evolving capillary
pressure gradient) itself, which in turn is a function of the
contact angle, rendering a complicated dependence of the ls
on roughness-wettability coupling.
Central contribution of this paper is a generalization in
the description of a DSL characterizing imbibition of water
molecules through nanopores. To assess the universal charac-
teristic of this generalization, we have tested that our descrip-
tion of a dynamic slip accurately represents the capillary
filling dynamics of water through nanopores, even when the
simulation conditions based on which the generalized expres-
sion has been derived differ from the model conditions of a
dynamically filled-up capillary environment in which the
model is tested (except for the model data that are exclusively
specific to the description of water as a fluid). As a conse-
quence of this exercise, we have come to a conclusion that
the description of a DSL, as a combined function of a dimen-
sionless acceleration, roughness, and wettability parameter, is
a unique signature of the fluid under concern (all results col-
lapse to a single master curve plotted based on reduced pa-
rameters). This allows one to utilize the resultant functional
description of DSL in terms of a unique dimensionless accel-
eration parameter as a fundamental constitutive relationship
for the given fluid-substrate combination, which eliminates
the need of repeatedly executing expensive molecular dynam-
ics (MD) simulations for capturing capillary filling dynamics
of water through nanopores, and essentially a universal DSL

0003-6951/2012/101(15)/153112/5/$30.00 101, 153112-1 C 2012 American Institute of Physics

V

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 153112-2 C. Bakli and S. Chakraborty
description coupled with a pseudo-continuum formulation
will suffice.
Our simulation system for capillary filling consisting of
a reservoir containing water molecules that is connected to a
capillary with wall atoms is described using LJ potential (for
details, see supplementary material16). The length scale is
normalized using the LJ parameter r and time scale is nor-
qffiffiffiffiffiffiffiffiffi
malized using the reference parameter s ¼ 48k mr2
, where m
BT
being mass of a water molecule and kB being the Boltzmann
constant. The justification of our selection of system dimen-
sions comes from the analysis of adsorption isotherms which
demonstrate that typical naturally occurring nano-porosities
(for example, consider the capillary phenomena occurring in
zeolites and clay pores) are of the length scales of 3 nm or
less. We choose the wall thickness greater than 3r to exclude
the thin wall effects. We specify the heteronuclear interac-
tions using a modified LJ potential, with parameters varied
to tune the surface roughness and wettability characteristics.
A random roughness function is used (see supplementary
material16) and is chosen to mimic the molecular interactions
due to surface roughness characteristics without explicitly
generating rough surfaces from a geometrical perspective.17
In the representation of this roughness function, N is a param-
eter that quantifies the extent of roughness (lower the value of
N, rougher the surface is). We calculate heteronuclear interac-
tions using Lorentz-Berthelot mixing rule.18 For interactions
involving water, we augment the LJ potential to incorporate
electrical and polarization potentials, conforming to SPC/E
model.19 We choose rWW ¼ 0:35 nm, and vary eww from 2 to
6 (corresponding to an equivalent contact angle variation
from 75 to 0 ). We use a modified Nose-Hoover thermostat-
ing technique20 (for details, see supplementary material16), so
as to constrain the wall molecules at T ¼ 300 K. We restrain
the wall atoms to their mean positions using springs with
sufficiently large spring constants, in effort to limit their vibra-
tions below a threshold value.21 The best possible comparative
idea, closest to a real system, can be drawn from the flexible
thermostatted walls.22 We average the data over several simu-
lation runs to generate robust, smooth, and reproducible menis-
cus filling characteristics. We determine the meniscus location
by tracking abrupt depletions in number density of water from
its bulk value (for details, see supplementary material16).
Based on the above-mentioned simulation environment,
we obtain MD predictions on water imbibition through nano-
pores of varying roughness and wettability characteristics. It
is, however, important to note that the focus of this work is
not merely to describe the corresponding MD simulation
results, but to demonstrate that those may be effectively repro-
duced by a LW model in a remarkably universal manner,
based on a fundamental, consistent, and generalized descrip-
tion of the DSL. The remaining part of this paper, therefore,
centers on the derivation of a consistent constitutive model for
DSL, which effectively enables one to achieve this feat.
Towards fulfilling the above objectives, it may be men-
tioned that one way of obtaining the DSL variation data may
be to utilize the data obtained from MDS of the capillary fill-
ing process itself, so as to train the LW model with a fitted
variation of ls that essentially mimics the same MD data
based on which the mentioned fitting is executed. This
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Appl. Phys. Lett. 101, 153112 (2012)
approach, however, does not remain far from being question-
able, primarily because of the fact that it fails to depict the
intricacies of the underlying physics by being “forced” to
mimic the same data by which it is inherently trained. In
addition, use of such a consideration may potentially over-
look the physics of a dynamically varying pressure gradient
in a capillary. This stems from the fact that for a given capil-
h
lary pressure drop, ð2ccosR Þ the pressure gradient across the
capillary evolves dynamically, as the capillary gets progres-
sively filled. Interestingly, for the length scales addressed in
this work, one may encounter dramatically large values of
the instantaneous driving acceleration that is a function of
the instantaneous capillary pressure gradient, which, in turn,
is inversely proportional to the length of the capillary already
been filled. Further, it can be shown that the driving accelera-
tion is inversely proportional to the capillary radius. Their
combined consequences, in effect, ensure dramatically large
acceleration values encountered in the filling of capillaries of
reduced dimensions as addressed in this work, for which the
slip length itself is a function of the driving acceleration.
Clearly, an estimation of the underlying consequences by
merely fitting the corresponding MD data itself leads to a
physics-free type of analysis, as attributable to its inherent
incapabilities in flushing out the relevant controlling parame-
ters and obtaining their functional dependences in a universal
form.
In an effort to characterize the DSL as a combined func-
tion of the driving acceleration, the contact angle, as well as
the surface roughness characteristics, we perform completely
independent sets of non-equilibrium molecular dynamics
(NEMD) simulations that are based on liquid-filled channels
(characterized with different surface wettabilities and rough-
ness features) of different lengths (essentially mimicking
snapshots of instantaneous liquid columns of various lengths
in a continuously filled capillary), with driving accelerations
imposed that are compatible with the typical capillary pres-
sure gradients (for more details of our NEMD simulations on
filled-up channels, see supplementary material16). We obtain
the slip/stick lengths from the respective velocity profiles.
We take the water-specific simulation data for NEMD simu-
lations to be identical to that corresponding to the ones
employed for the capillary filling simulation data. We ensure
that the filled-up channel simulations address all possible
ranges of driving acceleration to which a nanopore being
continuously filled may be effectively subjected, so as to
arrive at a universal depiction of the DSL. This leads to a
comprehensive constitutive description of the DSL charac-
teristics based on capillary-filling-independent MD data, as
depicted in Fig. 1, in which the variation of ls with surface
wettability, ranging from a partially to completely wettable
substrates, is shown for different values of the volumetric
driving force (conforming to the Laplace pressure gradients
in the capillary) as realized through an acceleration parame-
ter, a ¼ ccos h
qRL , and expressed in terms of its dimensionless
form a ¼ cRcos
gLdL
h
. The plots depicted in Fig. 1 reveal that for
dt
any particular roughness condition (fixed value of N), ls is
not only a function of h, but also depends on a. One may
note in this context that the driving acceleration  pR2pRc
2 LðtÞq,
where LðtÞ is the instantaneous length of the capillary
 153112-3 C. Bakli and S. Chakraborty
that has already been filled. Considering c  101 N=m;
R 109 m; q103 kg=m, LðtÞ  109 m, we obtain that
aðtÞ  1012 m=s2 (please note the R1 and LðtÞ
1
dependence of a).
Such high values of the driving acceleration during transients
of the capillary filling, in conjunction with some exclusive
characteristics of water as a polar fluid (as explained in details
later) indeed, are responsible for a strong acceleration-
dependence slip length. Since the acceleration itself evolves
dynamically during the capillary filling process, the slip
length also appears to be dynamically evolving. Such dynam-
ically evolving large acceleration values are intrinsic to capil-
lary filling processes over the scales considered in this work,
but are not normally encountered in experiments concerning
filled-up nanochannel flows. In addition, it is remarkable to
mention that the ls data depicted in Fig. 1 reveal the following
generalized form of functional dependence (for a given sur-
face roughness characteristic) on the dynamically evolving
A1 ðaÞ
acceleration: ls ¼ ð1þcos hÞ2
 A2 ðaÞ, where A1 ðaÞ and A2 ðaÞ
1 eration dependent slip length trends; the polar nature of the
are functions a. Importantly, the ð1þcos hÞ2
-dependence, though
elusively heuristic, may actually be postulated based on
physically based scaling arguments; for details, see Ref. 23. It
is interesting to note that as the driving acceleration is
changed, the curves shift vertically. However, this vertical
translation along the slip/stick axis can be observed for
extremely high shear values24–33 which may be often difficult
to practically generate in a filled channel flow. Although such
magnitudes of acceleration are quite common, as shown
above in the scaling analysis, in channel filling flows for the
length scales under consideration. With lower values of accel-
eration, our results approach the quasi-universal slip
description.23
Further to the above considerations, we have also stud-
ied the behavior of polar fluids in comparison to reduced flu-
ids, towards assessing their relative implications on dictating
the DSL characteristics. Notably, we have observed through
our simulations that the effect of acceleration-dependence of
slip length turns out to be inconsequential towards dictating
the capillary filling dynamics of LJ fluids (our results, in this
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Appl. Phys. Lett. 101, 153112 (2012)
FIG. 1. Slip lengths (normalized with respect to
channel height) obtained from independent
NEMD simulations in filled-up channels of
varying wettability, corresponding to different
values of a dimensionless acceleration parame-
ter, a . Bold lines represent the closet fits con-
1
sidering ð1þcoshÞ 2 -based functional dependence.
Inset (right) shows the variation of slip length
with inverse of the acceleration (m/s2) values
typically encountered in a capillary filling envi-
ronment over the spatio-temporal regime con-
sidered. Inset (left) shows the normalized ls
plotted against non-dimensional acceleration
a . Irrespective of the details of the underling
roughness-wettability-driving force coupling,
the dimensionless slip lengths converge to a
single universal curve (see inset (left); in which
scattered points represent NEMD data). S in the
legend represents smooth wall.
regard, corroborate the findings of Dimitrov et al.9 and we
demonstrate the filling behavior in Fig. 2 for a fluid which
have properties similar to water except for the fact that the
interactions are represented using only LJ potentials at the
oxygen sites). However, simulations with water in SPC/E
model demonstrate the driving acceleration dependence of
slip/stick length. This essentially stems from the fact that
water, as a polar fluid, exhibits unique dynamical features in
its stick-slip characteristics. Water molecules moving on the
wall-induced bumpy energy landscapes form local depleted
and/or concentrated structures owing to their own charge dis-
tribution and polarization. Moreover, each water molecule
creates its own potential imprint affecting other water mole-
cules. The inclusion of these additional features in the
description of interaction potential leads to cooperative
strengthening of such intermolecular structures formed by
water molecules. Our simulation data have revealed that
high driving acceleration during transients of a capillary fill-
ing process is not alone responsible for producing the accel-
fluid and the associated interfacial structuration also contrib-
ute to the observed behavior.
Proceeding further, we next attempt to capture a univer-
sal functional variation in the nanopore filling characteristics,
by devising a more generic functional dependence of ls, for
water. In order to obtain such a constitutive relationship in
its most general form, we first recast the DSL in terms of the
non-dimensional acceleration parameter a , defined as
a ¼ cRcos
gLdL
h
, which physically represents the ratio of scales of
dt
the driving capillary force to the retarding viscous force.
Remarkably, the variations in ls exhibit a unique functional
dependence on the dimensionless parameter a , for any com-
binations of roughness-wettability and the driving accelera-
tion (see left inset of Fig. 1). It is also important to mention
in this context that the dependence on the surface roughness
characteristics, though not apparent from the functional de-
pendence delineated as above, is rather implicit, and may
best perceived through a modification in the normalized
acceleration, so that a rough ¼ a smooth þ a. Here, a essentially
acts like a deceleration parameter, mimicking hindered
 153112-4 C. Bakli and S. Chakraborty
capillary filling characteristics triggered by rough surfaces.
Interestingly, a is observed to be an exponentially decaying
function of the roughness parameter N (for the range of sim-
ulation data covered in this work, this specific functional de-
pendence turns out to be: a ¼ 0:35 expð0:6NÞ, within an
error of 61%). It is also important to mention that we have
also verified that the present model merges asymptotically
with the models reported in the literature9,11,13,14 that con-
form to low-enough values of the acceleration parameter, so
that ls ceases to become sensitive to the driving acceleration
any more, as comprehensively verifiable from the right inset
depicted in Fig. 1.
Interpreting Fig. 1 for its further implications towards
analyzing capillary filling dynamics over pertinent physical
scales, the NEMD data for liquid-filled channels are essen-
tially mapped on to a capillary that may be perceived to be a
dynamic compilation of progressively evolving snapshots of
liquid-filled columns, considering a dynamically evolving
acceleration parameter a ðtÞ as the meniscus advances. Sub-
stituting the DSL variation depicted in Fig. 1 (left inset) in
the LW expression, following the above spirit, gives simple
analytical estimates of the capillary filling characteristics,
which are depicted by solid lines in Fig. 2. The ideal LW
behavior for a completely wetting capillary wall is shown by
the dashed line. The property values for SPC/E water used to
obtain the LW prefactor are calculated from standard consid-
erations34,35 and match quite well with the experimental val-
ues. Interestingly, it is revealed that the solid lines in Fig. 2
closely capture the corresponding MD predictions (colored
markers), despite not being trained from the same MD data.
The generalized equations obtained explain the gradually
decreasing value of the slope of the L2 versus t characteris-
tics. This behavior has been observed in reported simula-
tions9,12–14 as well as benchmark experiments.10,36 Using
artificial fitting parameters, this deviation has often been
absorbed in the form of an extra dL dt term with the traditional
LW equation, claiming it to be the contribution of DCA.12
However, the observed behavior is in contradiction to that
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Appl. Phys. Lett. 101, 153112 (2012)
FIG. 2. MD results (identified by markers, cor-
responding to various contact angles) depicting
the meniscus dynamics in a capillary being con-
tinuously filled as a function of time, with the
roughness parameter N ¼ 4 (as an illustrative
example). The dashed straight line depicts the
LW dynamics without slip for completely wet-
ting capillary wall which matches with the capil-
lary rise of LJ fluids. The bold lines depict the
predicted behavior obtained by solving the LW
model coupled with the universal DSL based
closure model, approximated in the forms of lin-
ear fits. The inset, as a representative scenario,
depicts the simulation data and one-dimensional
predictions (with our DSL model) corresponding
to nanopores with varying roughness character-
istics, corresponding to h ¼ 45 . S in the legend
represents smooth wall.
explained by DCA. Both the hydrodynamic theory and the
molecular kinetic theory15 for DCA predict more favorable
contact angles with progressive advancement of the menis-
cus, which is opposite to the dynamical characteristics
obtained through MD simulations reported here. Obtaining
the contact angles directly from the simulation data also sug-
gests that the contact angle relaxes to the static value within
a very short time span. This essentially suggests that DCA
does not play any significant role over the spatio-temporal
scales addressed in this work.
It is extremely important to emphasize at this point that
the simulation paradigms for the NEMD studies on filled up
channel and MD studies on a capillary that is being continu-
ously filled, as reported here, are conceptually different. In a
capillary that is being continuously filled, the slip lengths
cannot be calculated as these flows are inherently unsteady.
These two entirely different systems, nevertheless, are
intrinsically linked via a common universal stick/slip length
characteristic that is a single-valued function of a . Notably,
we execute the NEMD simulations on filled up channels
with the sole purpose of arriving at a universal description of
the DSL. Once arrived at, the history of obtaining such a
description no more remains relevant, and same functional
depiction of the DSL, may be employed for capturing the
imbibition dynamics of a capillary even with consideration
of different model configurations, provided that the same
fluid is under concern.
To summarize, we have derived a universal analytical
depiction of capillary imbibition characteristics of water in
nanoscale pores, through the realization of a molecularly
sensitive closure model for DSL (as verified by extensive
MD simulations), so that a simple one-dimensional force bal-
ance model can capture the underlying intricacies. Such
advantages in the modeling paradigm may bear far-ranging
scientific and technological consequences in designing mini-
aturized devices following the modern-day advancements in
nanotechnology, as well as understanding various geo-
physical and bio-chemical processes.
 153112-5 C. Bakli and S. Chakraborty Appl. Phys. Lett. 101, 153112 (2012)

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