LIQUID CRYSTALS AND POLYMERS

https://doi.org/10.15407/ujpe63.2.150

V.M. MYHAL,1 O.V. DERZHKO 1, 2

1 Ivan Franko National University of Lviv, Chair of Theoretical Physics
(12, Dragomnov Str., Lviv 79005, Ukraine; e-mail: vasylmyhal@ukr.net)
2 Institute for Condensed Matter Physics, Nat. Acad. of Sci. of Ukraine

(1, Svientsitskyi Str., Lviv 79011, Ukraine; e-mail: derzhko@icmp.lviv.ua)

WETTING UNDER ELECTROMAGNETIC

RESONANCE IRRADIATION

The influence of the resonance electromagnetic irradiation on the wetting of a solid surface by
liquid has been discussed. A simple model of a fluid consisting of two-level atoms, for which
changes in their interaction due to a resonance irradiation can be found in the framework of
the quantum-mechanical perturbation theory is considered, and the corresponding functional
for the grand thermodynamic potential is found. The density functional method is used to
calculate the surface tension at the liquid–vapor, solid–liquid, and solid–vapor interfaces, and
the Young equation is applied to determine the wetting angle. It is shown that the resonance
irradiation can significantly increase the latter parameter.
K e y w o r d s: resonance irradiation, density functional method, surface tension, wetting angle.

1. Introduction cited electron state is much longer than the equi-

The study of the solid surface wetting by a liquid librium establishment time in the system by means
is important from both the theoretical and practical of the translational degrees of freedom. As a re-
viewpoints [1–4]. They say that a liquid wets a solid sult, the fluid reveals equilibrium properties at a
surface, if the Young equilibrium wetting angle 𝜃, given concentration of excited atoms [14–22]. On the
i.e. the angle between the liquid and solid surfaces un- other hand, there appear new effective long-range
der thermodynamic equilibrium conditions, tends to (resonance dipole-dipole) interactions in a system
zero, and that it does not do it if 𝜃 tends to 180∘ . The composed of identical atoms in different electron
wetting angle can change, if external parameters (e.g., states. They can change the macroscopic equilibrium
the temperature) are varied. The density functional properties of the system, even if the concentration
method [5–13] makes it possible to study the depen- of excited atoms is low [14–31]. In this connection,
dence of 𝜃 on external parameters proceeding from a a number of experimental studies concerning fluids
microscopic picture, because it allows the properties under a resonance irradiation conditions can be men-
of an inhomogeneous liquid to be calculated on the tioned [32–42].
basis of particle-particle interactions. The microscopic theory of a fluid consisting of two-
In this work, the atomic fluid under a resonance level atoms was proposed in our works [23–31]. This
electromagnetic irradiation is considered. The radia- theory makes it possible to analyze the influence of an
tion frequency corresponds to the energy of atomic external electric field or resonance irradiation on such
excitation, so that some atoms can be in the ex- macroscopic equilibrium properties of a non-uniform
cited electron state. The lifetime of atoms in the ex- system as the binodal, spinodal, coefficient of surface
tension, and nucleation barrier for the vapor–liquid or
○
c V.M. MYHAL, O.V. DERZHKO, 2018 liquid–vapor phase transitions. In our works, we used
150 ISSN 2071-0194. Ukr. J. Phys. 2018. Vol. 63, No. 2
 Wetting under Electromagnetic Resonance Irradiation

)︃
the density functional method both in the mean-field −1 + 6𝑣𝜌(r1 ) − 4𝑣 2 𝜌2 (r1 )
approximation and going beyond it. + , (2)
(1 − 𝑣𝜌(r1 ))2
In our recent work [43], we studied the effect of
an external electric field on the wetting angle for where 𝜇 is the chemical potential, Λ the thermal
a two-level atomic liquid. In this work in a similar de Broglie wavelength, and 𝑣 = 𝜋𝜎 3 /6. The second
way, we considered the resonance irradiation effect term in Eq. (1) takes the long-range interaction into
[14–22]. The structure of the work is as follows. First account. The pair distribution function 𝜌(2) (r1 , r2 )
of all, the choice of a functional for the grand ther- looks like
modynamic potential, which depends on the concen-
tration of excited atoms, is discussed. The express- 𝜌(2) (r1 , r2 ) ≃ 𝜌(r1 )𝜌(r2 ) (3)
sion obtained for the grand thermodynamic potential in the mean-field approximation. The attractive part
makes it possible to find the surface tension, and, af- of the long-range potential of pair interaction is given
terward with the use of the Young equation, the equi- by the formula (see works [20–22])
librium wetting angle 𝜃. The results obtained demon-
strate that the growth in the concentration of excited 3𝜎 3 𝑎 1
𝑈 (r1 , r2 ) = 𝑈 (|r1 − r2 |) = − . (4)
atoms increases the wetting temperature 𝑇𝑤 , i.e. the 2𝜋 |r1 − r2 |6
temperature, at which 𝜃 vanishes (cos 𝜃 = 1), and in-
If there are excited atoms, the coefficient 𝑎 depends
creases the wetting angle 𝜃 at a fixed temperature.
on the concentration of atoms in the excited state, 𝑐1 ,
Moreover, it can transform the complete wetting into
and the temperature 𝑇 as follows:
a partial one and even stimulate the transition from
the hydrophilic to hydrophobic state, when cos 𝜃 be-
𝑣(𝐸1 − 𝐸0 )𝛼2
(︂ )︂
𝐸1 − 𝐸0
comes negative. 𝑎= 1 − 2𝑐1 + 2(1 − 𝑐1 )𝑐1 ,
32 𝑘𝑇
2. Density Functional Method (5)

When developing the theory of an inhomogeneous where 𝐸1 − 𝐸0 is the energy of two-level atom ex-
fluid consisting of two-level atoms [23–31, 43], we citation, 𝛼 = |p|2 /(𝜎 3 (𝐸1 − 𝐸0 )) is a dimensionless
use the density functional method [5–7]. The short- parameter characterizing the atom, and |p| the mag-
range repulsion was taken into account in the local nitude of the electric dipole moment for the transition
approximation, which corresponds to the Carnahan- between the ground and excited states of the atom
Starling equation of state for hard balls, whereas the (see works [20–22]).
long-range interaction was considered in the nonlocal The equation for the equilibrium density 𝜌(r) is
approximation. Let us start from the following func- obtained from the condition 𝛿Ω[𝜌(r)]/𝛿𝜌(r) = 0 [5–
tional for the grand thermodynamic potential [23–31]: 13] and looks like [23–31, 43]
)︀ 8𝑣𝜌(r) − 9𝑣 2 𝜌2 (r) + 3𝑣 3 𝜌3 (r)
(︂ )︂
(︀ 3
Ω[𝜌(r)] = 𝐹CS [𝜌(r)] + 𝑘𝑇 ln Λ 𝜌(r) + +
(1 − 𝑣𝜌(r))3
∫︁
1
∫︁
+ dr1 dr2 𝜌(2) (r1 , r2 ) 𝑈 (r1 , r2 ) + + dr1 𝜌(r1 )𝑈 (|r1 − r|) + 𝑉 (r) − 𝜇 = 0. (6)
2
|r1 −r2 |≥𝜎 |r1 −r|≥𝜎
∫︁
For a homogeneous fluid (𝜌(r) = 𝜌 and 𝑉 (r) = 0),
+ dr1 𝜌(r1 )(𝑉 (r1 ) − 𝜇). (1)
the equation of state in terms of dimensionless vari-
ables reads
The first term in this expression makes allowance for
the short-range repulsion between hard balls with di- 𝜋 1 + 𝜂 + 𝜂2 − 𝜂3 𝑎(𝑐1 , 𝜏 ) 2
=𝜂 3 − 𝜂 .
ameter 𝜎 written in the Carnahan–Starling form: 𝜏 (1 − 𝜂) 𝜏

∫︁ (︃ Here,
𝛼2
(︂ )︂
𝐹CS [𝜌(r)] = 𝑘𝑇 3
dr1 𝜌(r1 ) ln(Λ 𝜌(r1 )) + 2(1−𝑐1 )𝑐1
𝑎(𝑐1 , 𝜏 ) = 1−2𝑐1 + , (7)
32 𝜏
ISSN 2071-0194. Ukr. J. Phys. 2018. Vol. 63, No. 2 151
V.M. Myhal, O.V. Derzhko

0,0032
of a semiinfinite flat solid surface to 𝑉 (𝑥, 𝑦, 𝑧) = 𝑉 (𝑧)
at 𝑧 ≥ 𝜎 is calculated by integrating the interatomic
interaction −3𝜎 3 𝑎/(2𝜋𝑅6 ) [see Eq. (8)]. As a result,
0,0028
we obtain

𝑉 (𝑧) = 𝜌𝑠 ×
0,0024

∫︁∞ ∫︁∞ ∫︁0 √︁

′ ′
× d𝑥 d𝑦 d𝑧 ′ 𝑈 ( 𝑥′ 2 + 𝑦 ′ 2 + (𝑧 − 𝑧 ′ )2 =
0,0020 −∞ −∞ −∞

𝜌𝑠 𝑎 𝜎 3 1
=− . (8)
0,0016 4 𝑧3
0,0 0,1 0,2 0,3 0,4 0,5

Fig. 1. Binodals in the density–temperature plane for various Hereafter, for convenience, we put 𝜂𝑠 = 𝜌𝑠 𝑣 = 1.
concentrations of excited atoms 𝑐1 = 0 (solid curve), 0.00006 Additionally, we put 𝑉 (𝑧) = ∞ at 0 ≤ 𝑧 < 𝜎.
(dashed curve), and 0.0001 (dotted curve) Substituting the solution of Eq. (6) for the equi-
librium density into Eq. (1), we obtain the required
𝜋 = 𝑝𝑣/(𝐸1 − 𝐸0 ) is the dimensionless pressure, 𝜏 = expression for the grand thermodynamic potential of
= 𝑘𝑇 /(𝐸1 − 𝐸0 ) is the dimensionless temperature, the inhomogeneous system, Ω.
and 𝜂 = 𝑣𝜌 is the dimensionless density. Hereafter,
for simplicity, we put 𝛼 = 1 1 .
3. Results and Their Discussion
From Eq. (7), it is easy to determine the critical
parameters – namely, the critical density, tempera- The wetting angle 𝜃 is determined as follows. Firstly,
ture, and pressure – and to plot the corresponding the liquid-vapor surface tension 𝛾𝑙𝑣 is calculated. We
phase diagram (see Fig. 1). Since the parameter 𝑎 in put 𝑉 (r) = 0 in Eq. (6) and find a solution for the
Eq. (7) depends on the concentration of excited atoms equilibrium density 𝜌(𝑧) depending on the height 𝑧.
𝑐1 , the critical temperature 𝜏𝑐 and the critical pres- Substituting this solution into formula (1), we obtain
sure 𝜋𝑐 also depend on 𝑐1 . an expression for the grand thermodynamic poten-
Now, we have to know the explicit expression for tial of a two-phase fluid, Ω. The surface tension 𝛾𝑙𝑣 is
the external potential 𝑉 (r) that describes the inter- determined from the relation Ω = Ω0 + 𝛾𝑙𝑣 𝑆, where
action between the solid surface (substrate) and the Ω0 = −𝑝𝑉 is the grand thermodynamic potential for
atoms in the liquid. For simplicity, we assume that the homogeneous system in the volume 𝑉 (the pres-
a continuous solid surface, 𝑧 < 0, is formed by uni- sure in the system is 𝑝 in this case), and 𝑆 is the
formly distributed two-level atoms with the density interphase surface area.
𝜌𝑠 . Those atoms interact with the environment of The surface tension at the solid-liquid, 𝛾𝑠𝑙 , or solid-
two-level atoms by means of the same potential as in vapor, 𝛾𝑠𝑣 , interface is calculated in the framework of
the fluid (see, e.g., works [46–48]) 2 . The contribution the same scheme, but the interaction potential 𝑉 (r)
(8) has to be taken into consideration at that. We
1 Of course, for real atoms, the value of 𝛼 differs from unity. assume that the interface is located at 𝑧 = 0. While
For instance, for the 1𝑠2 − 1𝑠2𝑝 transition in a He atom, calculating 𝛾𝑠𝑙 (or 𝛾𝑠𝑣 ), we put the liquid (vapor) den-
𝐸1 − 𝐸0 ≈ 21.27 eV, |p|2 /𝜎 3 ≈ 0.15 eV, so that 𝛼 ≈ 0.007. sity at 𝑧 to be equal to the corresponding value at
At the same time, for the 6𝑠2 − 6𝑠6𝑝 transition in a Ba 𝑧 → ∞, i.e. 𝜌(𝑧) = 𝜌𝑙 or 𝜌(𝑧) = 𝜌𝑣 , respectively. Af-
atom, 𝐸1 − 𝐸0 ≈ 2.24 eV, |p|2 /𝜎 3 ≈ 0.94 eV, and 𝛼 ≈ terward, we determine the equilibrium density 𝜌(𝑧)
≈ 0.420. For those calculations, we used data from [44]
for all 0 ≤ 𝑧 < ∞, the grand thermodynamic po-
(see also work [45]). The analysis of parameter for other
systems, which would be of interest for experimental studies,
tential Ω, and, finally, the value for 𝛾𝑠𝑙 or 𝛾𝑠𝑣 . The
is outside the scope of our work. wetting angle 𝜃 is determined from the Young equa-
2 If the solid wall is formed by uniformly distributed two-level tion
atoms located in the plane 𝑧 = 0, we obtain the dependence
𝑉 (𝑟) ∼ 1/𝑧 4 rather than 𝑉 (𝑟) ∼ 1/𝑧 3 as in Eq. (8). 𝛾𝑠𝑣 − 𝛾𝑠𝑙 − 𝛾𝑙𝑣 cos 𝜃 = 0. (9)
152 ISSN 2071-0194. Ukr. J. Phys. 2018. Vol. 63, No. 2
 Wetting under Electromagnetic Resonance Irradiation

1,0

cos
0,8

0,6

0,4

0,2

0,0

-0,2

-0,4

0,55 0,60 0,65 0,70 0,75 0,80 0,85 0,90 0,95 1,00 1,05

T/Tc(c1=0)
Fig. 3. Dependences of cos 𝜃 on the concentration of excited
Fig. 2. Dependences of cos 𝜃 on the temperature 𝑇 /𝑇𝑐 (𝑐1 = 0)
atoms 𝑐1 at various temperatures 𝜏 = 0.9574𝜏𝑐 (𝑐1 = 0) =
for various concentrations of excited atoms 𝑐1 = 0 (squares),
= 0.00282 (squares), 𝜏 = 0.9𝜏𝑐 (𝑐1 = 0) = 0.00265 (circles),
0.00006 (circles), and 0.0001 (triangles)
and 𝜏 = 0.8𝜏𝑐 (𝑐1 = 0) = 0.00236 (triangles)

160
This is a final stage of finding 𝜃(𝑇, 𝑐1 ) from the first -6
(1-cos ) x10
principles, i.e. proceeding from the interparticle inter- 140
actions modified by the resonance irradiation. The re-
120
sults of calculations are depicted in Figs. 2 and 3. The
temperature dependence of the wetting angle exhib- 100
ited in Fig. 4 satisfies the relation 80

1 − cos 𝜃 ∝ (𝑇𝑤 − 𝑇 )2−𝛼𝑠 60

40
with 𝛼𝑠 = 1, which corresponds to the wetting phase
transition of the first order [49]. 20
Let us discuss the results obtained. In the case of
0
a fluid of two-level atoms, the presence of excited 0 2 4 6 8 10
atoms increases the long-range attraction. As a re- (( Tw-T)/Tc(c1=0)) x10 -6

sult, the critical temperature of the liquid increases: Fig. 4. Dependence of 1 − cos 𝜃 on the temperature (𝑇𝑤 −
𝑇𝑐 (𝑐1 ̸= 0) > 𝑇𝑐 (𝑐1 = 0). Hence, after the irradiation − 𝑇 )/𝑇𝑐 (𝑐1 = 0). The dependence 1 − cos 𝜃 ∝ (𝑇𝑤 − 𝑇 )2−𝛼𝑠
has been “switched-on” at a constant temperature, with 𝛼𝑠 = 1 describes the phase transition of the first kind.
the two-phase state “turns out” farther from the crit- The dependences for three different concentrations of excited
ical region. The surface tensions 𝛾𝑠𝑙 and 𝛾𝑠𝑣 increase atoms 𝑐1 lie on the same straight line: 𝑐1 = 0 (squares), 0.00006
(circles), and 0.0001 (triangles)
with the concentrations of excited atoms. If 𝛾𝑠𝑙 grows
more rapidly than 𝛾𝑠𝑣 , cos 𝜃 may can change its sign
in accordance with formula (9), and the hydrophilic a bit lower than the complete wetting temperature
surface (cos 𝜃 > 0) becomes hydrophobic (cos 𝜃 < 0). 𝑇𝑤 < 𝑇𝑐 , even a low concentration of excited atoms
We adopted a very simple model for the sub- 𝑐1 can induce noticeable changes of 𝜃 (see the curve
strate. The external potential 𝑉 (r) can be smaller, for 𝜏 = 0.00282 in Fig. 3).
e.g., owing to the reduction of 𝜂𝑠 . In this case, the To summarize, we applied the density functional
substrate role decreases: it remains hydrophobic even method to a simple fluid of two-level atoms in or-
in the absence of excited atoms. The wetting angle der to study the influence of the external irradiation
increases with the concentration of excited atoms on the wetting properties. The corresponding theo-
𝑐1 . If the temperature is very close to but remains retical analysis could describe liquid droplets that
ISSN 2071-0194. Ukr. J. Phys. 2018. Vol. 63, No. 2 153
V.M. Myhal, O.V. Derzhko

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