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ISSN No. 2454-6194 | DOI: 10.51584/IJRIAS |Volume X Issue IX September 2025
Design of Uniform Spray Nozzle and Simulation of Carrier Gas Flow
Rate Distribution for FTO Thin Film Fabrication Process
HyeSuk Ri, SongHyok Han, NamChol Yu*, GiWon Yang, GwangRyong Choe
Faculty of Electronics, Kim Chaek University of Technology, Pyongyang, Democratic People’s Republic
of Korea
*Corresponding Author
DOI: https://dx.doi.org/10.51584/IJRIAS.2025.100900096
Received: 16 August 2025; Accepted: 23 August 2025; Published: 25 October 2025
ABSTRACTS
The FTO thin films were deposited on 15 cm × 15 cm glass substrates by ultrasonic spray pyrolysis and the
influence of process parameters on the film properties was investigated. This paper is the first report on the
design of a uniform nozzle and simulating the carrier gas flow characteristics in an ultrasonic spray pyrolysis
process. The uniformity of FTO films was evaluated by surface resistivity. The structure, surface morphology
and optical properties of FTO films were investigated using scanning electron microscopy, X-ray diffraction,
and UV-Vis spectroscopy. The process conditions for film preparation were SnCl4 concentration of 1.34 mol,
NH4F concentration of 0.08 mol, temperature of 500 °C, deposition time of 15 min, carrier gas flow rate of 3
m/s, distance between nozzle and substrate of 0.7 cm. The transmittance of the fabricated FTO films was 80%,
the surface resistance showed a uniform behavior at 14-15Ω/and the X-ray analysis showed a high
orientation of SnO2 crystals in the 200-plane. SEM analysis showed that the crystallite size was constant.
Keywords: Nozzle; Design; FTO film; Simulation; Ultrasonic spray pyrolysis
INTRODUCTION
Transparent conductive films have been widely used in solar cells [1] or thermal-reflective glass [2,3]
optoelectronic devices [4,5] due to their high transmittance in the visible and near infrared regions and high
reflectivity in the far infrared regions.
To improve the electrical conductivity and transmission properties of transparent conductive films, tin oxide is
doped with In and Sb [6], F [7], Ce, Fe [8], Mn [9] Co [10], Mo [11], rare earth elements Pr [12], Nb [13], Ce
[14], La [15], Pd and Nb.
Among these impurities, fluorine added from ammonium fluoride (NH4F) is the most commercially available
because of its low cost and simple processing.
There are several methods for preparing transparent conductive films, such as the spray pyrolysis method [18,
19] and the chemical vapor deposition method, such as the sol-gel method [16, 17].
Many researchers have prepared FTO thin films under different process and reaction conditions and
investigated the electro-optical properties.
Bogle et al. [22] used spin-coating technique to obtain FTO films, with resistivity varying from 1.01×103 to
7.3×103Ω/cm. The thin film doped with Gd in SnO2 layer was obtained by Adjimi [23], using spray pyrolysis
technique, in which the resistivity decreased from 1.94×10-3 to 1.02×10-3/cm when Gd was added to SnO2 at
0-3%. Banyamin et al. [24] prepared FTO films using magnetron sputtering technique and their analysis
showed that the charge carrier concentration of undoped FTO films was 5.5×1018/cm3, while the charge
carrier concentration in the doped case was 1.46×1020/cm3. Yadav et al. [25] prepared SnO2:F films by
changing the substrate temperature using atomization technique, where the charge carrier concentration
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decreased from 3.63×1018/cm3 to 0.98×1020/cm3 when oxygen vacancies decreased at high temperature.
Kumar et al. [26] coated FTO films with NSP method, where the mobility increased from 15.88 m2V-1s-1 to
37.23 m2V-1s-1 with increasing solvent volume. Elangovan et al. [27] found that the maximum carrier
mobility for FTO film thickness of 1.2 lm is 24.7 m2V-1s-1.
Among various deposition methods, spray pyrolysis or atmospheric pressure chemical vapor deposition have
the advantage of low cost of thin film fabrication.
The reported properties of FTO films prepared using spray pyrolysis and atmospheric pressure chemical vapor
deposition are shown in Table 1.
Table 1. Surface resistance, transmittance resistance, quality factor and deposition method of FTO films
fabricated under different conditions.
Rs(Ωsq
-1
) T(%) ρ×10-
4
(Ωcm) Haze value Deposition routes Reference
6.5
70
7.0
Spray Pyrolysis
[16]
10.0
75
4.5
Spray Pyrolysis
[17]
4.4
80
3.3
Spray Pyrolysis
[18]
4.0
78
2.7
c-AACVD
[19]
18.0
70
APCVD
[20]
23.3
78
3.7
APCVD
[21]
75
6.9
APCVD
[22]
40.0
88
13.0
Pulsed Laser
[23]
Among these deposition methods, ultrasonic spray pyrolysis is a simple and cost-effective film deposition
technique [36]. This method is a method of obtaining a target metal oxide film by spraying a metal salt
solution containing the components of the film to be obtained using an ultrasonic transducer and then
pyrolyzing it on a substrate heated with a carrier gas such as air [37]. The advantage of this method is that the
ultrasonic nebulizer can obtain a uniform droplet of micrometer size and the initial velocity of the produced
droplets is small, so that the pyrolysis reaction of the film can be more stable by controlling the carrier gas
flow rate. Also, the low deposition temperature and precursor solvent used for film preparation are low cost
due to the use of alcohol or distilled water [38]. Also, the low deposition temperature and precursor solvent
used for film preparation are low cost due to the use of alcohol or distilled water.
In the process of thin film fabrication by ultrasonic spray pyrolysis, the design, rational structure and process
parameters of spray nozzle, which are the main process parameters to achieve the uniformity of the thin film,
are still poor in comprehensive analysis and consideration.
In this study, a novel spray nozzle was designed to fabricate homogeneous FTO films by ultrasonic spray
pyrolysis, and based on simulation analysis of flow rate distribution in the nozzle, FTO films were prepared
and compared with previous works.
Experimental
Ultrasonic spray pyrolysis process design
As reported in the literature, ultrasonic spray pyrolysis unit consists of spray process, nozzle feed process,
heating process and exhaust process [20, 21]. Fig. 1 is a schematic diagram of an ultrasonic spray pyrolysis
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unit. The ultrasonic sprayer has a working frequency of 1.7 MHz and a power of 180 W, with six piezoelectric
oscillators. The nozzle material is a stainless steel material with respect to its reactivity with the precursor
solution.
Fig. 1. Schematic diagram of ultrasonic spray pyrolysis unit.
Fig. 2 is the internal structure of the nozzle designed to provide sufficient mixing and uniform flow of the
spray
The nozzle inner structure has a 2.5cm cylindrical cavity with a pipe diameter size in the pipe joint, and from
this thickness it gradually narrows towards the discharge port.
The exit width is about 2mm and is mounted on the automatic feed device.
Fig. 2 nozzle design model
Precursor solution preparation
The glass samples of 15×15 cm in size and 3 mm in thickness were ultrasonically cleaned with acetone,
methanol and deionized water for 20 min to remove surface organics. As a precursor solution, 0.5 ml of
hydrochloric acid was added dropwise to a solvent mixed with 80% distilled water and 20 ethanol, and stirred
for 3min with a magnetic stirrer. Then, 1.34 mol of SnCl4•5H2O (98%) was added to the mixture, and after
complete dissolution, 0.08 mol of NH4F (98%) was added and stirred again for 20 min with a magnetic stirrer.
The stirred solution was filtered through a filter paper.
The prepared precursor solution was sprayed in an ultrasonic nebulizer.
The carrier gas uses air heated to 60 °C. The glass substrate temperature in the heating furnace was 500 °C and
kept for 15 min to account for the heat loss during film deposition. The spray nozzle moving speed, which is
set at 45° angle to the automatic feed, is 13 cm/s. The deposition time of the film was 15 min.
measurement analysis
XRD measurements were performed on an X-ray diffractometer (designation D8-ADVANCE, source CuKa
line, scan range 0°-80°, scan rate 0.06/S). The optical transmittance of FTO films was measured by UV-Vis
spectrophotometer (UV-160). The surface morphology of FTO films was measured by high-resolution SEM
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(Sign QUANTA 200). To evaluate the uniformity of the film, the organic substrate was divided into several
parts and the surface resistance was measured. The surface resistance (Rsh) was obtained from the four-probe
method by measuring the current (I) between two external probes, the potential difference (V) between the two
internal probes and the following equation [36].
Rsh =4.532(V/I) (1)
The coefficient 4.532 is applied to probes with a uniform 1 mm spacing of 1 cm × 1 cm sample size and a film
thickness smaller than the spacing between probes.
RESULTS AND DISCUSSION
Simulation of the uniformity of carrier gas flow rate in spray nozzle
Fig. 3 shows the simulation results with FLUENT 6.3 for the flow rate distribution when the airflow rate of the
carrier gas in the nozzle is varied from 3 to 6 m/s. The boundary condition is the density of the spray solution
1.293 kg/m3, the spray particle diameter is 1.94357 m, and the flow of carrier gas is turbulent flow mode. As
shown in the figure, the larger the carrier gas flow rate, the smaller the interval with uniform flow rate
gradually becomes. The reason is thought to be that the flow rate inside the nozzle increases with increasing
carrier gas velocity, thereby creating pressure due to carrier gas flow inside the nozzle. When the carrier gas
flow rate is less than 3m/s, the pressure inside the nozzle decreases and the uniform velocity distribution region
increases, but due to the close proximity of the heated substrate and the low carrier gas flow rate, the tin oxide
crystals are produced inside and outside the nozzle than the substrate. This leads to a decrease in the deposition
efficiency of the film on the substrate. Of course, when looking at the nozzle and substrate after FTO film
deposition, it can be seen that white crystals are deposited, which is seen as SnO2 crystals. Hence, the flow
rate of air carrier gas in the spray nozzle was set to 3 m/s.
Fig.4 shows the results of the FLUENT simulations analyzed at a flow rate of 3m/s of air carrier gas. As shown
in the simulation figure, the uniform velocity distribution is 17cm. Since the glass substrate is 15cm in size and
the uniform velocity distribution is 17cm, this region is acceptable when the FTO film is deposited with the
designed spray nozzle.
Fig. 3 Modeling of the distribution of carrier gas flow at different velocities
Fig. 4 Simulation results of FLUENT analysis at a flow rate of 3 m/s of air carrier gas
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To verify the accuracy of the results analyzed above, we are carried out the basic experiments for FTO thin
film preparation to evaluate the homogeneity of the films by surface resistivity measurements. Our basic
experiments for the film homogeneity evaluation were performed by ultrasonic spray pyrolysis using the
precursor solution and the experimental method described previously. Figure 5 shows the measured surface
resistance values of the FTO film and several split points fabricated.
Fig.5 Surface resistance values measured on fabricated FTO films and several indexing points.
As can be seen, the surface resistance of the fabricated transparent conductive film is 14-15Ω/ and only
17Ω/ in one edge. This is expected because the film deposition efficiency was reduced due to heat loss at the
edge of the organic substrate. The above results were also confirmed by SEM and X-ray diffraction analysis
showing the microstructure and crystal morphology of the films.
Fig. 6 SEM images of FTO thin films
As shown in Fig. 6, the grains with a clear shape and shape are uniformly distributed throughout the whole
area. This is expected to contribute to the uniformity of the nozzle, although the crystal size produced during
the basic experiments is constant and the surface resistance values are larger than those reported in previous
studies. In addition, the XRD results of Fig. 7 showed significant crystallinity on the 200, 211, 110 and 310
planes, as reported in the literature [39]. The high intensity of the 200-plane diffraction is likely to be
dominated by the crystal growth of the FTO film in the 200-plane direction due to the fluoride impurity effect.
This behavior is consistent with the data reported in the literature.
Fig. 7 X-ray diffraction data of fabricated FTO thin films
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Therefore, it is thought that the designed spray nozzle is effective for deposition of uniform FTO film and the
obtained film also has good characteristics as FTO film.
Effect of carrier gas flow rate
Based on the simulation results of the flow rate of carrier gas, a characterization of the flow rate of carrier gas
was carried out. At that time, surface resistance change is shown in Fig. 15.
Fig. 8 Changes in membrane surface resistance with carrier gas flow rate
In Fig. 8, the film surface resistance decreased and then showed an increasing trend with increasing carrier gas
flow rate. At a carrier gas flow rate of 1 m/s, the membrane surface resistance was very high, with a maximum
value of 104 Ω/, gradually decreasing from 2 m/s to 8 Ω/ at 3 m/s, and slightly increasing from the central
part at 4 m/s to 5 m/s. Also, as the carrier gas flow rate increased, the nozzle shape was significantly different
in the surface resistance characteristics due to the non-uniform film thickness at the center and edge of the
substrate. The film was homogeneous when the carrier gas flow rate was less than 3 m/s, but the surface
resistance was very high, and the difference was almost as severe as 10-50 Ω/when the carrier gas flow rate
was higher than 3 m/s. When the carrier gas flow rate was 1 m/s, the transmittance of the film showed a
maximum transmittance of 88% in the visible region, and 80% in the visible region at 3 m/s. The lowest
transmission in the 350 nm wavelength range was found at a carrier gas flow rate of 5 m/s. At a constant jet
distance, the carrier gas velocity of 1 m/s was such that the atomized fogs were pyrolyzed and nucleated and
evaporated by heat convection, without overcoming the upward convective flow due to the substrate thermal
energy and reaching the substrate. Hence, the film formation rate and efficiency were low, and only the grains
with large grains were attached to the substrate, which increased the transmittance and surface resistance
properties. On the other hand, when the carrier gas flow rate was around 5 m/s, the spray particle collided with
the substrate at a high rate and increased the nucleus and crystal growth attached to the substrate for a unit
time, resulting in an increase in particle size, thereby decreasing the film transmittance and surface resistance
in the visible region.
Effect of distance between substrate and spray nozzle
To study the effect of the distance between the substrate and the spray nozzle, the distance between the nozzle
and the substrate was varied from 0.5 to 1.1 cm, and the pyrolysis temperature was set at 500 °C, carrier gas
flow rate of 3 m/s and deposition time was set at 15 min using the precursor solution described previously.
Based on these process parameters, the morphology, light transmittance and surface resistance of the fabricated
FTO films were measured. Fig. 9 shows the variation of transmittance and surface resistance with the distance
between the substrate and the spray nozzle.
Fig. 9 Transmittance and surface resistance variation with the distance between substrate and spray nozzle.
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In the figure, as the distance between the spray nozzle and substrate increased, the transmittance changed
linearly with the slope greatly, and the surface resistance changed smoothly. The lower nozzle substrate
distance increased the heat loss of the substrate by spraying the adherent substrate. This is likely due to the
growth of the crystalline particles that have not been fully pyrolyzed on the substrate, which does not allow for
rapid replenishment of the lost heat. Also, if the distance between the substrate glass heated at high
temperature and the spray nozzle was too close, the substrate was damaged due to thermal shock of the
substrate. It can be seen that the distance between the spray nozzle and the substrate with excellent electro-
optic properties is between 0.5 and 0.9 cm.
Changes in the electrooptical properties of FTO films with the concentration of spray solution
Fig. 10 shows the surface resistivity and transmittance profiles of FTO films with respect to the stannous
chloride concentration. As can be seen in Fig. 10, the surface resistance of the transparent conductive film
gradually decreases with increasing the concentration of tin chloride. From the graph in Fig. 10, the
relationship between the concentration of tin chloride (N) and the surface resistance is expressed as Eq. 1.
Rsh= 5.3275N0.803 (2)
L² = 0.9453
Here L is the squared error between the functional expression and the measured value.
Through this square error value, the functional expression can be approximated to correspond to the
relationship between surface resistance and stannous chloride concentration.
Fig. 10 Surface resistance of FTO films with stannous chloride concentration
Fig. 11 Transmittance profiles of FTO films with stannous chloride concentration
As the concentration of tin chloride increases, the lattice defects increase due to the substitution of Cl atoms in
the SnO2 lattice. The decrease in surface resistance and transmittance is due to the increase in crystallinity of
the films.
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Effect of fluorine impurity
Table 1 shows the change in surface resistance with stannous chloride concentration and doping amount and
average transmittance variation in the range of 300-800 nm.
Table 2. Variation of properties with stannous chloride concentration and doping
SnCl
4
,
M
Impurity
Concentration,0.027
mol
Impurity
concentration,
0.054mol
Impurity
concentration,
0.08mol
Impurity
concentration,
0.1mol
Impurity
concentration,
0.135mol
R
sh
,Ω/
T, %
R
sh
,Ω/
T, %
R
sh
,Ω/
T, %
R
sh
,Ω/
T, %
R
sh
, Ω/
T, %
1.08
200
85
105
82
78
83
65
80
45
79
1.17
100
83
75
81
29
81
20
78
18
75
1.34
56
82
35.4
80
10.2
78
6.8
76
5.6
71
1.68
35
80
28.6
79
6.4
76
5.5
63
3.5
60
2.36
20
77
12.2
68
4.2
65
3.2
62
2.6
59
3.72
12
69
7.5
56
3.5
51
2.8
48
2
45
Table 2 shows low surface resistance to less than 10 /when the concentration of ammonium fluoride is
higher than 1.34 mol and the concentration of ammonium chloride is higher than 1.08 mol. This is due to the
increased charge carriers in the film crystals.
However, as the concentration of tin chloride and dopant increased, the average transmittance of the 300-800
nm wavelength decreased by 45%. The surface resistivity decreased with increasing concentration and doping
of stannous chloride and changed almost uniformly from 1.08 mol to more. The reason is that the amount of
fluorine atoms substituted with oxygen atoms in SnO2 crystals increases, acts as impurities and increases the
carrier scattering phenomenon, which leads to a decrease in charge carrier concentration and a larger crystallite
size [40, 41].
Also, the reason for the rapid decrease in average transmittance at 300-800 nm with the concentration of tin
chloride and dopant is thought to be due to the increase in the size of the crystal particles, which leads to the
increase in the film thickness, which leads to the transmission of light in this wavelength range, and thus to the
reflection or scattering [42].
CONCLUSIONS
A spray nozzle was designed to prepare FTO thin films by ultrasonic spray pyrolysis process, the carrier gas
flow characteristics were simulated, and the film uniformity was evaluated by surface resistance. The process
conditions for the preparation of the films used in the experiments were: SnCl4 concentration of 1.34 mol,
NH4F concentration of 0.08 mol, temperature of 500°C, deposition time of 15 min, carrier gas flow rate of
3m/s, distance between nozzle and substrate of 0.7 cm. The transmittance of the fabricated FTO film was
around 80%. The prepared FTO films showed a uniform behavior with surface resistance between 14 and
15Ω/and X-ray analysis showed a high orientation of SnO2 crystals in the 200-plane. SEM analysis showed
that the crystallite size was constant.
Further investigation of the process in more detail is required to improve the transmittance and surface
resistance of FTO films based on the simulation of the homogeneous characteristics of the heating process.
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