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The Mathematics of
Moving Contact Lines in
,,
Thin Liquid Films
,,
Andrea L. Bertozzi
,,,,
The motion of a liquid under the influence of sur-
face tension is a phenomenon we experience every
day when we take a shower, drink a cup of coffee,
or turn on the windshield wipers. All of these real-
world situations involve not only the motion of the
liquid and surrounding air but also their interac-
tion with adjacent hard surfaces. As we know from
waxing our cars and cooking with nonstick cook-
ware, the dynamics of a fluid coating a solid sur-
face depend heavily on the surface chemistry.
Many industrial processes, ranging from spin coat-
ing of microchips to de-icing of airplane wings, rely
on the ability to control these interactions.
An ongoing challenge is to explain the under-
lying physics of the motion of a contact line, a
triple juncture of the solid/air, solid/liquid, and
liquid
θ
solid
air
well defined at the contact line because the limit interact with particles in the solid substrate via a
along the surface is zero, while the limit along the “nonretarded” potential. The references [13] and
liquid/air interface (which is moving) is nonzero. [20] and the references therein provide more dis-
Regardless of the liquid/air interface model, the cussion of this and other potentials.
tangential component of force exerted by the fluid The lubrication approximation can be derived
on the solid diverges whenever the velocity is mul- from a systematic rescaling and asymptotic ex-
tivalued at the contact line [14, 18]. pansion of the Navier-Stokes equations in the limit
The fact that such a paradox exists is hardly sur- of vanishing capillary number Ca and Reynolds
prising. We should not expect to find a self-con- number Re , two dimensionless parameters given
sistent universal hydrodynamic model that does by
not incorporate the surface chemistry. Several 3νV ρV h0
models have been proposed to study the motion (4) Ca = , Re = ,
γ ν
of moving contact lines. All of them involve adding where ν is viscosity, γ is surface tension, and V
an additional effect on a microscopic length-scale. is the characteristic velocity of the film. The result
The two that we discuss in the next paragraphs are is the dimensionless lubrication equation
(1) weakening the no-slip boundary condition via
a slip condition effective at small scales and (2) in- ht + ∇ · (f (h)(∇∆h − ∇g(h))) = 0,
corporating the effect of long-range “Van der Waals (5) f (h) = h3 + b3−p hp ,
forces” between the liquid and solid. g(h) = (Ca)1/2 h + CΠ(h).
Perhaps the simplest context in which to test
these theories is that of thin viscous coating flows. Here b represents a dimensionless slip length,
For such problems a lubrication approximation and C is a dimensionless parameter that depends
simplifies bulk flow fluid dynamics to a single on the Hamaker constant and the characteristic
equation, relating the depth-averaged horizontal height h0 of the film.
fluid velocity to the shape and thickness of the liq- Typically only a subset of the terms in the equa-
uid/air interface. The Navier slip condition2 near tion appear in any one given paper. For example,
the liquid/solid interface demands that the veloc- Greenspan [16] derives (5) with b > 0 , “singular
ity at the interface be proportional to its normal slip” p = 1 > 0, and Π(h) = 0 . Haley and Miksis
derivative: [17] consider this same model with different inte-
∂u ger values of p = 0, 1, 2 . Williams and Davis [24]
(2) u= k(h) at z = 0. study film rupture due to Van der Waals interac-
∂z
Here u is the vector-valued horizontal fluid velocity tions via an equation of the type (5) with b = 0 (no
and z is the variable in the direction normal to the slip) and the incorporation of Van der Waals forces
solid surface. The parameter k(h) is a slip para- (with Π < 0 ). In all cases the highest-order term in
meter and can depend on the thickness h of the the model describes fourth-order degenerate dif-
film. We can think of condition (2) as a general- fusion, a phenomenon we discuss in more detail
ization of the standard no-slip condition, which cor- in the next section.
responds to k ≡ 0 in (2). The engineering and applied mathematics lit-
Another choice for removing the singularity erature has had much discussion of the most ap-
due to no slip is to include microscopic scale propriate boundary conditions for an equation of
forces, in the form of long-range Van der Waals the form (5) near the vicinity of a contact line, es-
(VW) interactions between the liquid and solid sub- pecially in the context of a slip model.5 During the
stances, near the contact line. The most system- past eight years mathematicians working in the
atic way to do this is via an additional body force field of nonlinear PDEs have become interested in
in the fluid of the form3 this problem from a more analytical point of view.
In this article we explain some of the funda-
(3) Π(h) = AD hD−5 , mental mathematics problems associated with
where D is the dimension of the substrate.4 Here such equations as well as some of the rigorous ma-
AD is the Hamaker constant, depending on the di- chinery and numerical methods that have been
mension of space and also on the strength of the developed recently to attack these problems.
interaction between the liquid and solid particles.
The sign of AD depends on whether the VW forces Fourth-Order Degenerate Diffusion
are attractive or repulsive. The particular power in Diffusion equations arise in models of any physi-
(3) comes from assuming the particles in the fluid cal problem in which some quantity spreads or
smears out. The classical example is the heat equa-
2A generalization of the no-slip condition in which the fluid tion ht = ∇ · k∇h where the diffusion coefficient
is allowed to slip tangentially along the solid boundary. k controls the rate at which heat “diffuses” through
3As in §II.D of [13] and in §II.E of [20].
4That is,
D = 2 for a film on a two-dimensional surface 5See §§II.B and V of [20] and the references therein. See
and D = 1 for a flow in the plane, bounded by a line. also Hocking, J. Fluid Mech. 239 (1992).
the medium. In order to understand the models priori pointwise lower bound depending only on
proposed in equation (5) we need to understand the H 1 norm and minimum value of the initial data.
something about degenerate diffusion equations, This form of a weak maximum principle is due to
where the constant k depends on the solution u the nonlinear structure of (7), not the structure of
in a degenerate way, so that k → 0 as u → 0. A fam- the fourth-order diffusion operator. It is note-
ily of second-order degenerate diffusion equations worthy that other fourth-order degenerate diffu-
is known as the porous media equations [21]: sion equations with different nonlinear structure
have weak solutions that change sign (F. Bernis,
(6) ht − ∆(Φ(h)) = 0,
Nonlinear analysis and applications, 1987). De-
where Φ0 (h) > 0 for h > 0 and Φ(h) ∼ hm as h → 0. spite the positivity-preserving property for large
Here m > 1 makes the equation degenerate. n, solutions of (7) with smaller values of n com-
The Laplacian operator ∆ endows the evolu- putationally exhibit finite-time singularities of the
tion equation (6) with some well-known special form h → 0 . We discuss this phenomenon in more
properties: detail in the next section. The fact that such sin-
1. Instantaneous smoothing of the solution in re- gularities may occur makes the development of a
gions of positive h, since the equation is uni- weak solution theory, analogous to that of the
formly parabolic (i.e., the “diffusion coeffi- porous media equation, all the more difficult. Over
cient” is bounded away from zero) where the the past few years, mathematical machinery, largely
solution is bounded away from zero. involving energy estimates and nonlinear entropies,
2. Maximum principle. The solution is bounded have been developed to address these problems.
from above and below by its initial data. This Such methods have been used to prove weak max-
is true regardless of whether or not m = 1 imum principles, to derive existence results for
(heat equation) or m > 1 . weak (nonnegative) solutions, and to prove results
3. Well-posed weak solutions for smooth non- concerning the finite speed of propagation of the
negative initial data. support of nonnegative solutions (F. Bernis, 1996
4. Finite speed of propagation of the support of articles in Adv. Differential Equations and C. R.
the solution. Acad. Sci. Paris).
The last property is special to degenerate diffusion
( m > 1 ). The heat equation ( m = 1) has infinite
Finite-Time Singularities and Similarity
Solutions of Lubrication Equations
speed of propagation of the support.
Consider now the fourth-order analogue of (6), The study of finite-time singularities and similar-
ity solutions of (7) began in the early 1990s by a
(7) ht + ∇ · (f (h)∇∆h) = 0. group at the University of Chicago. The original pro-
In the context of thin film dynamics we are inter- ject addressed the breakup of a thin neck in the
ested in questions of existence, uniqueness, and “Hele-Shaw cell” when forced by external pres-
finite speed of propagation of the support of weak sures. The experiment, performed by Goldstein at
solutions of equations of the form (7). The im- Princeton [11], can be modeled, via lubrication the-
ory, by a fourth-order degenerate diffusion equa-
portant difference from the case (6) is that (7) is
tion in one space dimension:
fourth order as opposed to second order. It is dif-
fusive, so we have property (1), instantaneous (8) ht + (hn hxxx )x = 0
smoothing where the solution is positive; but prop-
erty (2), the maximum principle, is far from guar- with “pressure” boundary conditions h(±1) = 1 ,
anteed. Indeed, if we take the nondegenerate case hxx (±1) = −p , and n = 1. Carefully resolved nu-
f (h) = 1 , then solutions can change sign. This can merical computations revealed that this problem
be seen by simply examining the heat kernel for yields both finite and infinite time singularities for
fourth-order diffusion in RD and noting that un- various initial data.
like the well-known second-order heat kernel, the What is unusual about the structure of these sin-
fourth-order heat kernel has an oscillatory expo- gularities is that, while they locally have self-sim-
nentially decaying tail that changes sign. This be- ilar structure of the form
havior is illustrated in the color image shown on ³ ´
x − a(t)
the cover of this issue. It is not immediately ap- (9) h(x, t) ∼ τ(t)H ,
parent why the nonlinear problem (7) should have l(t)
solutions that preserve their sign. the time dependences τ, l(t), and a(t) are not de-
What is remarkable is that the nonlinear struc- termined by dimensional analysis of the PDE. Such
ture of (7) can endow it with a positivity-preserv- anomalous “second type” scaling [3] arises in prob-
ing property. In particular, one can show for one lems like the focusing solution of the porous media
space dimension for f (h) = hn with n ≥ 3.5 on a equation (Aronson and Graveleau, European J.
periodic spatial domain that if the initial condition Appl. Math. (1993)), where one solves a nonlinear
h0 is positive, then the solution h(x, t) is guaran- eigenvalue problem to determine the profile H
teed to stay positive. In fact, one can derive an a and the relationship between scales τ and l(t).
than n∗ allow for the possibility of finite-time sin- work [7] by Bernis and Friedman. There they
gularities. Critical exponents are also relevant for showed that, in addition to conservation of mass,
the weak solutions that continue the evolution Z
∂
after a “touch down” singularity or that evolve (11) h(x)dx = 0,
nonnegative initial data. Here the critical expo- ∂t
nent ncr it separates equations for which the so- and surface tension energy dissipation,
lution has increasing support from equations for Z Z
∂
which the support of the solution cannot increase. (12) |∇h|2 = − f (h)|∇∆h|2 dx,
For the porous media equation (6), the support of ∂t
the solution is always monotonically increasing, re- equations of the type (7) possess a nonlinear en-
gardless of the size of m > 1 . For the lubrication tropy dissipation of the form
equation (8) with D = 1, the support of the solu- Z Z
tion cannot increase whenever n ≥ 4 , as is shown ∂
(13) G(h) = − |∆h|2 dx.
in [6]. On the other hand, there are solutions with ∂t
support that eventually increase to fill the entire Here G(h) is a convex function satisfying
domain for all n < 3 . It has been conjectured that G00 (h) = 1/f (h). ForR the case f (h) = h (e.g.,
R Hele-
the critical exponent for increasing support is Shaw) the entropy G(h) is of the form h log h ;
ncr it = 3 , but this remains to be proved. hence the name “entropy” was born [9] to describe
The exact value of the critical exponent has im- this object. Using the entropy (13), Bernis and
portant ramifications for the moving contact line Friedman proved that in one space dimension the
problem. If indeed ncr it = 3 , it tells us that there critical exponent n∗ , above which singularity for-
are no solutions of (5) with b = 0 (no slip) that de- mation is forbidden, satisfies n∗ < 4 . The proof
scribe a moving contact line. Such a result would uses the fact that (12) and conservation of mass
not be surprising. It is consistent with the fact imply an a priori bound on the C 1/2 norm R of the
that such a scenario introduces a multivalued ve- solution while (13) insures a bound on h2−n . This
locity field that is known to produce infinities in gives an a priori pointwise lower bound for the so-
the physics (hence the introduction of the slip lution. R
terms that give n < 3 ). It turns out that the integral G(h)dx above is
Examples of known exact solutions support the not the only dissipative entropy. In one dimension
conjecture that ncr it = 3 in both one and two space we also have a family of entropies satisfying
dimensions. One class of examples is known as the Z
∂ hs
“source type solutions”, solutions that start as a (14) Gs (h) ≤ 0, (Gs )00 = ,
delta function at the origin and spread out in a self- ∂t f (h)
similar way while conserving their mass. Starov [22] where 12 ≤ s ≤ 1 . Taking s → 12 gave the upper
looked for such solutions to (7) with f (h) = h3 in bound n∗ ≤ 3.5 proved in [10].
two space dimensions. He was trying to find a sim- The generalized entropy plays an important
ilarity solution to describe spreading drops under role in the development of a weak existence the-
the influence of surface tension. What he discov- ory for nonnegative solutions from nonnegative ini-
ered was that the resulting ODE for the similarity tial data and for proving results on finite speed of
solution did not have any solutions of compact sup- propagation of the support. Uniqueness of weak
port. That is, there are no similarity solutions solutions still remains an open problem. Later in
describing spreading drops with no-slip on the this paper we see how entropies have also been
solid/liquid interface. Bernis and collaborators6 used recently to design numerical methods for
showed that in all space dimensions source type solving these equations.
solutions ( f (h) = hn ) exist for n < 3 and they cease
to exist for n ≥ 3 . What is interesting is that this Weak Solutions versus Constitutive Laws
critical exponent cannot be predicted from di- for Moving Contact Lines
mensional analysis of the equation; it is deter- The recent results on weak solutions of (7) have
mined by properties of the ODE for the shape of interesting ramifications for the moving contact
the similarity solution. Traveling wave (i.e., ad- line problem. Consider, for example, equation (5)
vancing front) solutions also change behavior at the with f (h) as given in (2) with b > 0 , 0 < p < 3 ,
critical exponent7 of 3. and g(h) = 0 . This particular model has been used
We now discuss some of the key ideas used to many times to describe motion of a moving con-
prove results about the PDE (7). A seminal paper tact line in either a partial wetting (where there ex-
in the mathematical development of the theory of ists an equilibrium configuration that locally solves
weak solutions for lubrication-type equations is the Young’s law (1)) or complete wetting context (where
the liquid energetically prefers to wet the solid).
6In Nonlinear Anal., TMA (1992), and European J. Appl. Greenspan and McKay considered this model with
Math. (1997). “singular slip” ( p = 1 ) and made an argument that
7Boatto et al., Phys. Rev. E. 48 (6) (1993). an additional boundary condition at the contact
line, in the form of a constitutive law, was required infinite speed of propagation of the support (as in
to obtain a well-posed model. Such conditions the case of regular, nondegenerate diffusion) as
make sense for nondegenerate fourth-order equa- well as the possibility of extinguishing of the so-
tions, but these arguments do not directly carry lution in finite time.
over to the general case where f (h) → 0 as h → 0 . In the case where Π(h) is positive (attractive
On a more physical level, we see that the con- forces) this could lead to a model where the su-
stitutive law and fixed contact angle models may perdiffusive term leads to some unphysical be-
make sense locally at a contact line, but they do havior for the solution. However, it turns out that
not address things such as topological transition, the model (3) for long-range Van der Waals inter-
i.e., what happens when two contact lines collide, actions is valid only on a mesoscopic length-scale,
or when a film ruptures and a new contact line that of 100–1000 Ångstroms. The model breaks
forms. down when the film reaches a molecular-scale
Recent progress has been made at constructing thickness. There are two ways of dealing with this
more robust models for certain specific cases. For breakdown of continuum theory: one is to use a
example, in the case of complete wetting we would modified continuum model with a cutoff of the sin-
like to construct a solution that has a zero contact gularity in (3) on a molecular scale. The other is to
angle and will eventually spread to cover the en- use a molecular model on this scale. In a 1994 ar-
tire surface. It was proved in [6, 9] that such a so- ticle in Nonlinearity, the author and Mary Pugh
lution does exist (for D = 1) for all slip conditions considered the former approach for the case of so-
(2) with 0 < p < 3 . The solution is for general H 1 lutions of (3) that depend on only one space co-
initial data and includes such phenomena as film ordinate. We showed that if one uses a “porous
rupture and droplet merger (see the computational media” type cutoff of (3), where the effective sec-
example in the next section). The method of con- ond-order diffusion coefficient behaves like the
struction is to use the weak maximum principle for nonlinear term in (6) with 1 < m < 2 , then there
such problems and to construct a positive solution exists a solution to (15) with support that eventu-
of a regularized problem (see, e.g., equation (18) ally increases to fill the domain and has, almost
below) and then pass to the limit in the regular- every time, a zero contact angle at the edge of the
ization parameter. These results have recently support. Numerical simulations of the model show
been extended to higher space dimensions.8 The that the “porous media” cutoff dominates the be-
higher-dimensional proof does not directly use havior of the solution at the edge of its support.
the regularization (18), since it does not guaran- A number of authors have performed simula-
tee positive approximations in more than one di- tions of molecular dynamics models of moving
mension. However, the recent existence results contact lines (see, e.g., [25, 23, 19]). However, the
are derived using higher-dimensional forms of the problem with a purely molecular model is that it
generalized entropies (14). is impossible to put enough particles in the sys-
Another recent manuscript by F. Otto proves the tem in order to see the interaction of the molecu-
existence of a fixed contact angle solution in one lar scale with macroscopic structures several or-
space dimension of (7) with f (h) = h . An interest- ders of magnitude larger than the molecular scale.
ing open problem is to try to extend this result to An interesting and difficult problem is the under-
prove existence of fixed contact angle solutions for standing of the interactions between these micro-
other slip models. scopic effects and the large-scale dynamics such
as surface tension.
Van der Waals Forces and Superdiffusion
The Van der Waals model with b = 0 and Numerical Methods for Solving Lubrication
g(h) = CΠ(h) also yields an interesting set of math- Equations
ematical problems. Here we consider models of the The complex structure of the fourth-order PDE
type poses a challenging problem for the design of nu-
merical methods for solving these problems. For
∂h
(15) = −div(h3 (∇(∆h − Π(h)))). the computation of nonnegative weak solutions, a
∂t
nonnegativity-preserving “finite element method”
The singularity in Π(h) (from (3)) yields an evolu- was proposed in [5]. This method allows for solu-
tion equation (15) that has fourth-order degener- tions with positive initial data to lose positivity; a
ate diffusion and second-order superdiffusion. variational problem involving a Lagrange multiplier
The latter refers to cases where the diffusion co- must then be solved to advance the nonnegative
efficient blows up as h → 0 . Superdiffusive prob- solution.
lems are known from [12] and the references Even when the analytical solution is strictly pos-
therein to have some strange behavior, including itive, the solution of a generic scheme may be-
come negative, especially when the grid is under-
8In Dal Passo et al., SIAM J. Math. Anal. 29 (2) (1998), and resolved. And once the numerical solution becomes
references therein. negative it cannot always be continued in time in
a unique or stable way. When a positive approxi- This idea can be generalized to an abstract fi-
mation of the solution is desired, it has been nec- nite-element setting. For positive solutions the
essary to do computationally expensive local mesh “entropy-dissipating” (EDS) finite-element method
refinement near the minimum of the solution in discussed in [26] differs from the one proposed in
order to avoid such premature or “false” singu- [5] only in that for the EDS scheme a nonlinear func-
larities [10]. Other examples include flow down an tion of the solution G0 (z) is assumed to be in the
inclined plane,9 where resolution was required at element space instead of the solution z itself and
the apparent contact line, and the approximation an additional numerical integration rule is im-
of nonnegative weak solutions via strong solu- posed. For solutions that lose positivity the scheme
tions [8]. in [5] requires solving a variational problem, while
Recent work of L. Zhornitskaya and the author EDS schemes are guaranteed not to lose positiv-
[26] shows that it is possible to use the entropy ity. We expect that the best choice of scheme will
depend on the specific problem of interest.
ideas above for smooth solutions of the PDE to con-
We now present a computational example from
struct numerical schemes that preserve positivity
[26] that illustrates the effectiveness of using a pos-
of the solution and hence have global solutions.
itivity-preserving (EDS) scheme over a generic one.
For example, consider a one-dimensional peri-
Consider the example discussed earlier with ini-
odic domain divided up into N equally spaced in-
tial condition (10) and n = 1/2 . We discussed the
tervals of size ∆x , with nodes x0 , . . . , xN. Let yi ap-
formation of a finite-time singularity that exhib-
proximate h(xi ), and denote by ited a discontinuiuty in third derivative as h → 0 .
yi+1 − yi yi − yi−1 From [7, 6, 9] we know that the solution can be con-
yx,i = , yx̄,i = , tinued in time as the limit of a sequence of posi-
∆x ∆x
yx̄,i+1 − yx̄,i yx̄x,i − yx̄x,i−1 tive approximations. That is, consider the regu-
yx̄x,i = , yx̄xx̄,i = larization
∆x ∆x
the finite differences in space. h²t + (f² (h² )h²xxx )x = 0,
The coupled system of ODEs
(18) h4² f (h² )
∂t yi + (a(yi−1 , yi )yx̄xx̄,i )x = 0, f² (h² ) = .
²f (h² ) + h4²
(16) i = 0, 1, . . . , N − 1,
yi (0) = h0 (xi ), Coarse Grid Computation. Generic Scheme.
is a continuous-time discrete-space approxima-
tion of the PDE
∂t h + ∂x (f (h)∂x3 h) = 0
h4²
f² (h² ) ∼ as h² → 0
²
Remarks
The contact line problem has generated some very
interesting and difficult mathematical problems as-
sociated with the model equations discussed in this
paper. In particular, questions of uniqueness of
weak solutions and the precise value of critical ex-
ponents remain rigorously unresolved. In the case
of critical exponents for finite-time pinch-off, it is
difficult even to conjecture what the correct value
might be. Much of the work on this particular as-
pect of the thin film equations is numerical, and
this work has shown what is probably just a small
subset of the kind of behavior that is possible for
solutions of higher-order degenerate diffusion
equations.
Figure 5: Comparison of computation in Figure 4 with We find that the dynamics of the moving con-
numerical solution on a fine grid. Same fixed time t = 0.001, tact line models can lead to complicated struc-
² = 10–11, ² = 10–13, and ² = 10–14; 1,024 grid points on [0,1]; ture of the solution in a neighborhood of the con-
log10 (min ∆t) = –6.7 for ² = 10–11, –7.0 for ² = 10–13, and –7.3 for tact line. Indeed, the complications associated with
² = 10–14. the models described here have led applied math-
ematicians to look at new formulations for re- [13] P. G. DE GENNES, Wetting: Statics and dynamics, Rev.
moving the singularity at the contact line [4]. Modern Phys. 57 (1985), 827.
It is the hope of the author that this article will [14] E. B. DUSSAN V and S. DAVIS, On the motion of a fluid-
fluid interface along a solid surface, J. Fluid Mech.
spark more interest in these problems within the
65 (1974), 71–95.
mathematical community which could lead to fruit- [15] SYDNEY GOLDSTEIN, ed., Modern developments in fluid
ful interactions with physicists and engineers work- dynamics, vol. 2, Dover, Inc., 1965.
ing in this field. [16] H. P. GREENSPAN, On the motion of a small viscous
droplet that wets a surface, J. Fluid Mech. 84 (1978),
Acknowledgments 125–143.
The author thanks Michael Brenner, Anthony [17] PATRICK J. HALEY and MICHAEL J. MIKSIS, The effect of
Knapp, and Mary Pugh for useful comments re- the contact line on droplet spreading, J. Fluid Mech.
223 (1991), 57–81.
garding this article. This work is supported by a
[18] CHUN HUH and L. E. SCRIVEN, Hydrodynamic model of
PECASE award from the Office of Naval Research
steady movement of a solid/liquid/fluid contact line,
and by a Sloan research fellowship. J. Colloid Interface Sci. 35 (1971), 85–101.
[19] JOEL KOPLIK, JAYANTH BANAVAR, and JORGE WILLEMSEN, Mol-
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100, Springer–Verlag, New York, 1994, pp. 155–208. bottom surface. Here we start with the same ini-
[11] PETER CONSTANTIN, TODD F. DUPONT, RAYMOND E. GOLD- tial data but evolve according to
STEIN, LEO P. KADANOFF, MICHAEL J. SHELLEY, and SU-MIN ht = −∇ · (h2 ∇∆h). Such degenerate diffusion
ZHOU, Droplet breakup in a model of the Hele-Shaw equations arise in models for moving contact
cell, Phys. Rev. E 47 (6) (1993), 4169–4181. lines, as discussed in this article, starting on
[12] PANAGIOTA DASKALOPOULOS and MANUEL DEL PINO, Re- page 689.
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