Journal of Alloys and Compounds 925 (2022) 166511

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Journal of Alloys and Compounds

journal homepage: www.elsevier.com/locate/jalcom

Synthesis chemical methods for deposition of ZnO, CdO and CdZnO thin
films to facilitate further research ]]
]]]]]]
]]

⁎ ⁎
B. Amudhavalli a, R. Mariappan b, , M. Prasath a,
a
Department of Physics, Periyar University PG Extension Centre, Dharmapuri 636 705, Tamilnadu, India
b
Department of Physics, Adhiyamaan College of Engineering, Hosur, Krishnagiri 635109, Tamilnadu, India

a r t i cl e i nfo a bstr ac t

Article history: Thin film materials have been used in semiconductor devices, wireless communications, telecommunica­
Received 20 October 2021 tions, integrated circuits, rectifiers, transistors, solar cells, lightemitting diodes, photoconductors and light
Received in revised form 25 July 2022 crystal displays, lithography, micro- electromechanical systems (MEMS) and multifunctional emerging
Accepted 26 July 2022
coatings, as well as other emerging cutting technologies. The ZnO, CdO and CdZnO thin films were de­
Available online 5 August 2022
posited by chemical routes such as chemical bath deposition, spray pyrolysis, Sol-Gel spin coating, elec­
trodeposition, SILAR, chemical vapour deposition, atomic layer deposition, and pulsed vapour deposition
Keywords:
Chemical route are discussed. Furthermore, the ZnO, CdO and CdZnO thin films depend on various preparative parameters
Metal oxides such as the molarity, pH of the solution, deposition time, annealing temperature, annealing time, thickness,
Thin films substrate used and pressure etc are also discussed.
Bath composition © 2022 Elsevier B.V. All rights reserved.
Film thickness

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ..... . ..... . ..... . ..... . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... . 2
2. Synthesis techniques for thin films deposition . . . . . ..... . ..... . ..... . ..... . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... . 2
3. Growth mechanism of deposited thin films . . . . . . . ..... . ..... . ..... . ..... . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... . 7
3.1. Chemical bath deposition method . . . . . . . . . ..... . ..... . ..... . ..... . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... . 7

Abbreviations: AlNO33, Aluminium nitrate; AlNO33.9 H2O, Aluminum Nitrate nanohydrate; AlNO33.9 H2O, Aluminum (III) nitrate nanohydrate; Al2O3, Aluminum oxide; Al2O3,
Aluminium oxide; AlCl3, Aluminium chloride; AuCl4·H2O, Gold(IV) chloride hydrate; AlCH33, Trimethylaluminum; AgNO3, Silver nitrate; CH3COOH, Acetic acide; CaCl2, Calcium
dichloride; CdCH3(COO2, Cadmium acetate; CdCH3COO2.2 H2O, Cadmium acetate dehydrate; CdCH3OO2.2 H2O, Cadmium acetate dihydrate; CdOH2, Cadmium hydroxide;
CdN2O6.4 H2O7, Cadmium nitrate; CdO, Cadmium oxide; CdSe, Cadmium selenide; Co CH3COO2.4 H2O, Cobalt (II) acetate hydrate; CO2, Carbon dioxide; Co3O4, Cobalt oxide;
CoCl2.6 H2O, Cobalt (II) chloride hexahydrate; CsBr, Cesium bromide; CuSO4, Copper sulfate; CuSO4.5 H2O, Copper sulfate pentahydrate; C2H6Cd DMCd, Dimethylcadmium;
C2H6OS, Diethylzinc, Dimethyl sulfoxide(C2H5)2 Zn (DEZn); CH2CH2OH2, Erythrosine, Diethanolamine (DEA)C20H6I4Na2O5·H2O; CH3CO23Er xH2O, Erbium (III) acetate hydrate;
CH2OH2, Ethylene glycol; CH26N4, Hexamethylenetetramine; C16H18CIN3S, Methylene blue; C6H12N4, Methenamine; C6H5NO3, Nitrophenol (4-NP); C2nH4n2 On+1, Polyethylene
glycol; C2F4n, Poly (Tetrafluoroethylene) (PTFE); C2H4Ox, Polyvinyl alcohol; C5O2H8, Poly (methyl methacrylate); C6H9NOn, Polyvinylpyrrolidone; C4H10O TBA, Tertiary butanol;
C4H8O, Tetrahydrofuran (THF); C6H18Al2, Trimethylaluminum (TMA); C7H8, Toluene; CH3CO23Y.xH2O, Yttrium (III) acetate hydrate; Cl2H2OZr, Zirconium (IV) Oxychloride; C11H8O2,
2-hydroxy-1-naphthaldehyde; C3H8O, 2-Propanol; ErNO33⋅5 H2O, Terbium (III) nitrate pentahydrate′; Eu2O3, Europium (III) oxide; EuCl3, 6 H2O, Europium (III) chloride hex­
ahydrate; EuH10N3O14, Europium nitrate pentahydrate; FeCl3, Ferric chloride; GaNO33•xH2O, Gallium (III) nitrate hydrate; Ga2O3, Gallium (III) oxide; GaCH33, Trimethylgallium;
H2O, Dihydrogen monoxide; H2, Hydrogen; HCl, Hydrochloric acid; H2SO4, Sulfuric acid; KCl, Potassium chloride; KOH, Potassium hydroxide; LaNO33.6 H2O, Lanthanum (III)
nitrate hexahydrate; LaCl3∙7 H2O, Lanthanum (III) chloride heptahydrate; MgNO32.6 H2O, Magnesium nitrate hexahydrate; MgO, Magnesium oxide; MnCH3COO2.4 H2O,
Manganese diacetate tetrahydrate; MnCl2.2 H2O, Manganese chloride dihydtrate; MoS2, Molybdenum disulfide; NH4CH3COO 0.2 H2O, Ammonium (II) acetate hydrate; NH4+,
Ammonium ion; NH4F, Ammonium fluoride; NH4NO3, Ammonium nitrate; NH4OH, Ammonium hydroxide; N2H4·H2O, Hydrazine hydrate; NbCl5, Niobium pentachloride; Nb
OCH2CH35, Niobium (V) ethoxide; NO2, Nitrogen dioxide; NO3, Nitrate; Na2S, Sodium sulfured; Na2S 0.9 H2O, Sodium sulfide Nonahydrate; Na2S2O3.5 H2O, Sodium thiosulfate;
Na2ZnOH4, Sodium zinc hydroxide; Na2ZnO2, Sodium zincate; NaBH4, Sodium borohydride; NaC12H25SO4, Sodium lauryl sulfate (SDS); NaC12H25SO4, Sodium dodecyl sulfate;
NaNO3, Sodium nitrate; NaOH, Sodium hydroxide; NCH2CH33, Triethylamine; OH, Hydroxide; PbNO32, Lead nitrate; PbBr2, Lead bromide; PrCl3.6 H2O, Praseodymium (III) chloride
hexahydrate; RuCl3.3 H2O, Ruthenium (III) chloride trihydrate; Sb2O5, Antimony; Sn [CH32N]4, Dimethylamino tin (IV); SrCl2.6 H2O, Strontium chloride; SmCl3, Samarium (III)
chloride; SiCH33, Trimethylsilyl; SnCl2.2 H2O, Tin (II) chloride dehydrate; SnO2, Tin oxide; TbNO33⋅5 H2O, Terbium (III) nitrate pentahydrate; Tm2O3, Thulium oxide; V2O5, Vandium
pentoxide; YCH3COO2.4 H2O, Yttrium (III) acetate tetrahydrate; Yb2O3, Ytterbium oxide; ZnCH3COO 2.2 H2O, Zinc nitrate, Zinc acetate dihydrateZn(NO3)2.6 H2O; ZnCl2, Zinc
chloride; ZnO, Zinc oxide; ZnSO4, Zinc sulfate; ZnSO4.7 H2O, Zinc sulfate heptahydrate; [ZnNH34]2, Tetraamminezinc (II) ion
⁎
Corresponding authors.
E-mail addresses: marijpr@gmail.com (R. Mariappan), sanprasath2006@gmail.com (M. Prasath).

https://doi.org/10.1016/j.jallcom.2022.166511
0925-8388/© 2022 Elsevier B.V. All rights reserved.
B. Amudhavalli, R. Mariappan and M. Prasath Journal of Alloys and Compounds 925 (2022) 166511

3.2. Spray pyrolysis method. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... . 10
3.3. Sol-Gel spin coating method. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... . 15
3.4. Electrodeposition coating method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... . 19
3.5. Successive ionic layer adsorption and reaction (SILAR) coating method . . . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... 21
3.6. Chemical vapor deposition method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... 23
3.7. Atomic layer deposition method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... 25
3.8. Pulsed vapor deposition method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... 28
4. Future opportunities for complex oxides. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... 30
5. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... 56
.................................................................. . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... 56
Declaration of Competing Interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... 56
Acknowledgments. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... 56
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ..... ..... . ..... . ..... . ..... . ..... . ..... . ..... . ..... 56

1. Introduction
The field of material science and engineering community’s ability
to conceive the novel materials with extraordinary combination of
chemical, physical and mechanical properties has changed the
modern society. Thin films are deposited by a wide range of coating
processes [1]. The deposition of materials begins this blog first with
the advantages of using thin films over the past decades due to
deposition processes applications such as engineering materials,
which are the future of thin-film technology. Engineered structures
developed from nano-wells, nano-wires, nano-tubes, nano-dots,
nano-composites, smart materials, photonic bandgap materials,
molecularly doped polymers, and structural materials can expand
and enhance the functionality of thin films and layers [2–15]. Thin
films are used in many applications and provide new applications.
New and combined advanced deposition processes are being used
and developed to deposit advanced thin-film materials and struc­
tures that were not possible with traditional methods a decade ago.
For example, until recently, it was important to store fully dense
films for all applications, but now engineering porous membranes
are finding many new uses. For example, hybrid processes that
combine asymmetrical magnetron sputtering and filtered cathode
arc deposition are producing thin-film materials at record hardness
[1,16,17].
Although the study of thin film phenomena dates back well over
a century, it is really only over the last four decades that they have
been used to a significant extent in practical situations. The re­
quirement of micro miniaturization made the use of thin and thick
films virtually imperative. The development of computer technology
led to a requirement for very high density storage techniques and it
is this which has stimulated most of the research on the magnetic
properties of thin films. Many thin film devices have been developed
which have found themselves looking for an application. In general
these devices have resulted from research into the physical proper­
ties of thin films. Thin film materials have already been used in
semiconductor devices, wireless communications, telecommunica­
tions, integrated circuits, rectifiers, transistors, solar cells, light-
emitting diodes, photoconductors, light crystal displays, magneto-
optic memories, audio and video systems, compact discs, electro-
optic coatings, memories, multilayer capacitors, flat-panel displays,
smart windows, computer chips, magneto optic discs, lithography,
micro- electromechanical systems and multifunctional emerging
coatings, as well as other emerging cutting technologies.
The Zinc oxide (ZnO) is an n-type semiconductor with versatile
applications such as optical devices in ultraviolet region, piezo­
electric transducers, transparent electrode for solar cells and gas
sensors. ZnO is normally n-type semiconductor at room temperature
with direct wide bandgap 3.25 eV. The CdO compound has a color of
reddish brown and is built by the process of burning of Cd in the air.
Cadmium oxide (CdO) gets an eminent popularity because of its
electrical and optical characteristics. In the application of electronic
device, thin films of Transparent Conducting Oxide (TCO) have great
acceptance. Among all of these TCOs, cadmium oxide (CdO) is an
ntype semiconductor which has a direct band gap at almost
2.2–2.7 eV. It is devoted to cover the most recent advances and re­
views the state of the art of ZnO and CdO thin films applications
involving energy harvesting, microelectronics, magnetic devices,
photocatalysis, photovoltaics, optics, thermoelectricity, piezo­
electricity, electrochemistry, temperature sensing. ZnO thin films
can be doped with variety of semiconductors to meet the demands
of several application fields. The ZnO and CdO thin films can be
deposited by variety of techniques, such as spray pyrolysis, sol–gel
method, filter vacuum (cathodic) arc deposition (FVAD, FCVD), suc­
cessive ionic layer adsorption and reaction (SILAR), electrodeposi­
tion, thermal evaporation technique and two-stage chemical
deposition (TSCD).
In this review article, we have tried to point out the important
key factors to be followed while depositing the chemical and phy­
sical properties of the ZnO, CdO and CdZnO thin films and their
applications.
2. Synthesis techniques for thin films deposition
The schematic diagram of the chemical bath deposition method
is shown in Fig. 1. [18] Chemical Bath Deposition (CBD), also called
Chemical Solution Deposition, is a method of thin-film deposition
(solids forming from a solution or gas), using an aqueous precursor
solution. Chemical Bath Deposition typically forms films using het­
erogeneous nucleation (deposition or adsorption of aqueous ions
onto a solid substrate), to form homogeneous thin films of metal
chalcogenides (mostly oxides, sulfides, and selenides) and many less
common ionic compounds. Chemical Bath Deposition produces films
reliably, using a simple process with little infrastructure, at low
temperature (< 100°C), and at low cost. Furthermore, Chemical Bath
Deposition can be employed for large-area batch processing or
continuous deposition.
Chemical bath deposition (CBD), an inexpensive growing method
that allows good quality thin-film semiconductors to be produced
over a large area and at low temperatures, is becoming the tech­
nology of choice. A metal complex is required for the membrane
growth of compounds II-VI in CBD. We have determined that the
stability constant (k) of a metal complex compatible with the CBD
growth mechanism is approximately 106.9. This value is low enough
to ensure that the complex adsorbed by the substrate expands to
react further with the chalcogen precursor. It is also high enough to
minimize the concentration of metal ions in the tank involved in the
precipitation of bulk solids. The homogeneous reaction leading to
precipitation in the reactor occurs because the solubility products of
II-VI compounds are in a very low bulk form. This reaction quickly
depletes the reagent bath, limits film thickness, and degrades film
quality [18,19]. Films produced by CBD are often used in semi­
conductors, photovoltaic cells, and supercapacitors, and there is

2
B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 1. The schematic diagram of chemical bath deposition method.
increasing interest in using Chemical Bath Deposition to create na­
nomaterials.
A nebulizer is a small machine that is powered by an air com­
pressor and can change the precursor solution into very tiny droplets
like mist. Though it is portable, it requires electric power to operate
the air compressor. Tubing connects the compressor to a cub of the
nebulizer that holds the liquid. The nebulizers use compressed air or
oxygen to break up a thin film or jet of fluid into droplets suitable for
deposition. The nebulizer bowl is filled with chemical in aqueous
solution or suspension. Compressed air or oxygen is applied to the
jet inlet and, traveling at a high velocity, exits through a narrow
orifice, creating an area of low pressure at the outlet of the adjacent
liquid feed tube. This pressure differential causes fluid from the re­
servoir to be drawn up into (i.e., the Venturi effect) and out of the
tube. The liquid is then shattered into droplets of various sizes by the
nebulizer walls or internal baffles. The larger droplets are returned
to the fluid reservoir, whereas the finer droplets are carried out of
the nebulizer to the glass plate by the flow of air. The experimental
setup of the nebulizer spray pyrolysis method is shown in Fig. 2. The
bottom of the vertical tube is designed carefully as a spray nozzle to
spray the chemical liquid mist on the substrate smoothly [20,21].
Fig. 2. The experimental set-up of nebulizer spray pyrolysis method.
3
Journal of Alloys and Compounds 925 (2022) 166511
Spin coating is a technique used to spread uniform thin films on
flat substrates by centrifugal force. The apparatus used for spin
coating is called a spin coater, or a spinner. A solution of material is
dispensed onto the center of a wafer, which is then rotated at high
speed. Rotation continues until the excess solution spins off the
substrate and the desired thickness of the film is left on the sub­
strate. The applied solvent is usually volatile and evaporates during
deposition. The two main factors that define film thickness are the
spin speed and the viscosity of the solution. Other factors considered
include spin time, solution density, solvent evaporation rate, and
surface wettability. For a typical case of photoresist deposition (e.g.,
AZ3312, viscosity 18 cP), rotation of 2000–6000 rpm is used for
30–60 s to obtain a 1.5–1 µm thick film. Soft baking (a drying process
at a relatively low baking temperature of ~ 100 °C) is usually per­
formed after deposition to evaporate the residual solvent and anneal
the mechanical stress. After the soft baking process, the photoresist
coating becomes photosensitive. Under-soft baking may leave a
considerable amount of solvent, which prevents exposure light from
reacting with the photoresist. On the other hand, over-soft baking
may reduce the resolution of photoresists by either changing the
developer solubility or damaging the resist.
Spin coating is one of the easiest ways to deposit various types of
materials that are in solution form. Deposition of polymers, nano­
particles, and biomaterials is commonly performed via spin coating.
Regardless of the materials that are deposited, spin coating usually
requires a drying or baking process [22]. The schematic diagram of
the sol-gel spin coating method is shown in Fig. 3 [23].
The successive ionic layer adsorption and reaction (SILAR)
method is one of the chemical methods for making uniform and
large-area thin films that is based on the immersion of the substrate
into separately placed cations and anions. The SILAR method in­
volves an alternative immersion of the substrate in a solution con­
taining a soluble salt of the cation and anion of the compounds to be
grown. The substrate supporting the growing film is rinsed in high
purity deionized water after each immersion in order to avoid
homogeneous precipitation. The interesting advantages and details
of the theoretical aspects of this method are thoroughly described in
B. Amudhavalli, R. Mariappan and M. Prasath Journal of Alloys and Compounds 925 (2022) 166511

Fig. 3. The schematic diagrams of Sol-Gel spin coating method.

the review by Pathan and Lokhande [24]. The SILAR method has
been successfully employed for many metal sulfides, selenides, and
tellurides, including oxides. As shown in Fig. 4, the beakers con­
taining precursor solutions and deionized water are alternately
placed. The immersion and rinsing of substrates are done manually
or using microprocessor-based systems [24,25].
The electrodeposition technique is used generally in electro­
plating and in the production of nano films. In this technique, two
electrodes (anode E1 and cathode E2 are immersed inside the elec­
trolyte as shown Fig. 5 [26,27].
When the current is passed through the electrolyte, certain mass
of substance is liberated from one electrode say for example from
electrode E1 and is deposited on the surface of the other electrode
say E2 and hence forms a thin nano film on the surface of the
electrode E2. The thickness of the nano film can be adjusted by
controlling the current and the time of deposition.
For example pure zinc (Zn) is taken as anode and another metal
or conducting material is taken as cathode. These two electrodes are
placed in ZnCl2 solution. When the current is passed through the
solution, the following reaction takes place.
ZnCl2 Zn+ + Cl2
Zn+ ion will move towards cathode and deposit on the surface.
Cl2 will get Zn+ liberated from pure zinc (anode). Thus the process
will continue till the current is passed through the solution.

Fig. 4. The schematic diagram of SILAR method.

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B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 5. The experimental set-up of electrodeposition method.
Chemical vapour deposition (CVD) is a technique that relies on
the formation of a gaseous species containing the coating element
within a coating retort or chamber. Alternatively, the gaseous species
may be generated external to the coating retort and introduced via a
delivery system. These gaseous species (eg, chromous chloride) are
then allowed to come into contact with the surfaces that require
coating. The retort is held at a high temperature, normally in excess
of 800 °C. The application of this thermal energy and the presence of
a reducing atmosphere results in the decomposition of the mole­
cules containing the coating element which are subsequently de­
posited onto the surface of the substrate. Using the CVD method a
wide variety of coatings may be formed, ranging from soft, ductile
coatings to those with hard, ceramic like properties. Coating thick­
nesses can vary from a few micron to over 200 mm, with hardnesses
in the range 150–3000 HV (0.1Kg). Coatings formed by the CVD
method are currently being used to combat the severe attrition of
components used in a variety of industrial situations where corro­
sion, oxidation or wear is experienced. The methods commonly used
to apply CVD coatings will be discussed and their advantages and
limitations examined. Several case studies will be highlighted,
where CVD coatings have been used to solve specific industrial
problems [28,29]. The schematic diagram of the Chemical vapour
deposition (CVD) method is shown in Fig. 6.
Fig. 6. The experimental set-up of chemical vapor deposition method.
5
Journal of Alloys and Compounds 925 (2022) 166511
Atomic layer deposition (ALD) is a vapor-phase technique used to
deposit thin films onto a substrate. The process of ALD involves the
surface of a substrate being exposed to alternating precursors, which
do not overlap, but instead are introduced sequentially. In each al­
ternate pulse, the precursor molecule reacts with the surface in a
self-limiting way. This ensures that the reaction stops once all of the
reactive sites on the substrate have been used. A complete ALD cycle
is determined by the nature of the precursor-surface interaction. The
ALD cycle can be performed multiple times to increase the layers of
the thin film, depending on the requirement. The process of ALD is
often performed at lower temperatures, which is beneficial when
working with fragile substrates, and some thermally unstable pre­
cursors can still be employed with ALD as long as their decom­
position rate is slow [25]. The process is shown in Fig. 7 [30,31]. A
wide range of materials can be deposited using ALD, including
oxides, metals, sulfides, and fluorides, and there is a wide range of
properties that these coatings can exhibit, depending on the appli­
cation. The ALD process is widely used as it provides ultra-thin nano-
layers in an extremely precise manner on a variety of substrates,
including micron to sub-micron size particles. The nano-layers
achieved with ALD are by nature conformal and pinhole free.
Fig. 8 depicts a schematic diagram of the PLD technique [32]. The
principle of pulsed laser deposition, in contrast to the simplicity of
the system set-up, is a very complex physical phenomenon. it in­
volves all the physical processes of laser material interaction during
the impact of the high-power pulsed radiation on a solid target. It
also includes the formation of the plasma plume with high energetic
species, the subsequent transfer of the ablated material through the
plasma plume onto the heated substrate surface and the final film
growth process. thus PLD generally can be divided into the following
four stages.
1. Laser radiation interaction with the target
2. Dynamic of the ablation materials
3. Decomposition of the ablation materials onto the substrate
4. Nucleation and growth of a thin film on the substrate surface
In the first stage, the laser beam is focused onto the surface of the
target. At sufficiently high energy density and short pulse duration,
all elements in the target surface are rapidly heated up to their
evaporation temperature. Materials are dissociated from the target
and ablated out with stoichiometry as in the target. The in­
stantaneous ablation rate is highly dependent on the fluences of the
laser irradiating on the target. The ablation mechanisms involve
many complex physical phenomena such as collisional, thermal and
electronic excitation, exfoliation and hydrodynamics. During the
B. Amudhavalli, R. Mariappan and M. Prasath Journal of Alloys and Compounds 925 (2022) 166511

Fig. 7. The schematic diagram of atomic layer deposition method.

second stage the emitted materials tend to move towards the sub­
strate according to the laws of gas-dynamic and show the forward
peaking phenomenon. The laser spot size and the plasma tempera­
ture have significant effects on the deposited film uniformity. The
target to substrate distance is another parameter that governs the
angular spread of the ablated materials.
The third stage is important to determine the quality of thin film.
The ejected High energy species impinge onto the substrate surface
and may induce various type of damage to the substrate. The me­
chanism of the interaction is illustrated in the following Fig. 8. These
energetic species sputter soma of the surface atoms and a collision
region is established between the incident flow and the sputtered
atoms. Film grown is immediately after this thermalized region
(collision region) is formed. The region serves as a source for con­
densation of particles. When the condensation rate is higher than
the rate of particles supplied by the sputtering, thermal equilibrium

Fig. 8. The experimental set-up of pulsed laser deposition method.

6
B. Amudhavalli, R. Mariappan and M. Prasath Journal of Alloys and Compounds 925 (2022) 166511

Table 1
Merits, demerits and applications of various deposition methods of thin films.

S.No. Deposition methods Merits Demerits Deposition Parameters Applications

1 Chemical bath
deposition
2 Spray pyrolysis
3 Sol-Gel spin coating
4 Successive ionic layer Save material cost, does not
adsorption and reaction require any capital and
(SILAR)
5 Electrodeposition
6 Chemical Vapor
Deposition
7 Atomic Layer deposition High quality films, control of the The time required for the
8 Pulsed Laser Deposition Conceptually simple, cost
Low cost, yields stable, uniform, Wastage of the solution after Bath composition, Deposition Blue diodes, flat displays, Layer for
easy set-up, Convenient Large every deposition temperature, time, annealing solar cells and gas sensors
area deposition, and good temperature and time, film etc.,[2,3]
reproducibility by a relatively thickness, stirring time, molarities,
inexpensive concentration of precursor
materials
Cost effective, Very efficient, It is not easy to scale-up (yield is Bath composition, molarities, Piezoelectricity,
utilizes simple equipment and very low), oxidation of sulfides Substrate temperature, spray rate, Photoconductivity, optical
large surface of coating. when processed in air pressure, time, pH, flow rate waveguides, and gas probes,
atmosphere is possible, and nozzle to substrate distance, etc.,[4,5]
Presence of impurities thickness and substrate used
Very simple, easy coating, low Wastage of deposition materials, Bath composition, molarities, Solar cell window layers, piezo-
cost, Better control of the less material efficiency concentration of precursor electric sensors, UV detectors,
structure, Extended composition materials, spinning speed and etc.,[6,7]
ranges, Better homogeneity and time, annealing temperature and
less energy consumption time, film thickness, and substrate
usded
High pressure needed Bath composition, Dipping speed Conducting layer in solar cells and
and time, substrate used, pH, optoelectronic devices, etc.,[8,9]
expensive instrument, Low thickness
deposition temperature, energy
saving, Deposition on large area
Low cost, large area growth, fast Limitation of thickness, Bath composition, pH, potential, Gas sensors, solar cells,
process, very good adherence, presence of impurities from current density, thickness, supercapacitor, corrosion,
good strength solvent substrate used, deposition time piezoelectric devices, and
and temperature batteries etc.,
Relatively high deposition rate, Applied a higher temperatures Microelectronics, solar cells, fuel
High purity (depending on the precursor), cells, batteries, LED, OLED,
difficult to mask surface, and etc.,[10,11]
size limited to reaction chamber
capacity.
Bath composition, Molarity, Capacitors, catalysts,
film thickness, high film density, chemical reactions, the deposition cycle, Annealing photoconductors, solar cells, Fuel
large area coating, low economic viability, very high temperature and time, film cells, etc.,[12,13]
temperature, Excellent adhesion material waste rate and very thickness and substrate used.
energy waste rate
Large kinetic energy, High laser Basic pressure, target substrate, High temperature
effective and very fast energies involved, working pressure, power density, superconducting thin films,
Annealed temperature and time, Optical coatings, Magneto-
film thickness, substrate used. resistive thin films, etc.,[14,15]

condition can be reached quickly and film grows on the substrate
surface at the expense of the direct flow of the ablation particles.
Nucleation and growth of crystalline films depends on many
factors such as the density, energy, degree of ionization, and the type
of the condensing material, as well as the temperature and the
physical chemical properties of the substrate [26–32]. The merits,
demerits, and applications of various deposition methods of thin
films are listed in Table 1.
3. Growth mechanism of deposited thin films
3.1. Chemical bath deposition method
The film formation mechanism is described by Tangade H.S. et al.
[33]. Chemical bath deposition (CBD) is based on the formation of a
solid phase from a solution, which involves two steps: nucleation
and particle growth. In the nucleation, the clusters of molecules
formed undergo rapid decomposition, and particles combine to grow
on the substrate surface. Zn(NO3)2 is used as a zinc source for the
deposition of ZnO film. When it was added to the above, it produced
a white precipitate of Zn(OH)2, which was dissolved by additional
ammonia. This can be represented by the following reactions [33]:
Zn (NO3)2 + 2NH4 OH Zn (OH)2 + 2NH4 NO3
Zn (OH)2 + 2NH4 OH (NH)4 ZnO2 + H2 O + H+
As the solution is heated, the ionic product exceeds the solubility
product and precipitation occurs on the substrate and in the solution
to form ZnO nuclei. ZnO film formation takes place as follows:
(NH)4 ZnO2 + H+ ZnO + ZH4 OH
However, due to the aqueous nature of the bath, the possibility of
Zn(OH)2 formation exists.
Low temperature synthesis of chemical bath deposited ZnO thin
films was achieved by Tangade H.S., et al. [33]. The diffraction pat­
terns of the X-ray diffraction characterization indicated that the
films were polycrystalline with a hexagonal wurtzite crystal struc­
ture. Fig. 9 represents the scanning electron micrograph of the ZnO
thin films at different magnifications. The lower magnification SEM
image shows the formation of flower like structure at some point. In
the higher resolution SEM images once can observe the rod shaped
structure is shown in Fig. 10. The wettability studies showed a water
contact angle of 91°, which confirms the hydrophobic nature of ZnO
thin films. Yumiyama R et al. [34] fabricated the ZnO film by in­
corporating erythrosine B dye molecules into a ZnO film. The re­
sultant hybrid film was transparent and coloured in red due to the
homogeneous distribution of the dye molecules. Such synergetic
electro/photochromic properties are relatively new and provide an
important insight into the design of chromic materials and de­
vices [35].
Sundararajan P., et al., developed the growth of one-dimensional
(ID) zinc oxide (ZnO) nano/micro rod arrays (N/MRAs) thin films by
using a facile, reproducible, and cost-effective method that could

7
B. Amudhavalli, R. Mariappan and M. Prasath Journal of Alloys and Compounds 925 (2022) 166511

et al., synthesized on glass substrates coated with an optimized Ga-

doped ZnO seed layer [37]. The TEM results show hexagonal NRs
which were aligned vertically on the substrate. At the 0.01 M Cs, the
mixture of tiny rods and agglomerated islands of particles wre ob­
served. With increase of Cs to 0.05 M, more reguar and orderly NRs
with improved morphology wre realized is shown in Fig. 11. The
reaction mechanism of ZnO thin film fabrication is described by
Muslih E.Y. et al. [38].
[Zn (NH3)4]2 + + H2 O Zn2 + + NH4 + + OH

Zn2 + + OH Zn (OH)2

Zn (OH)2 ZnO + H2 O

The chemical reactions during the growing process are explained

by Rosado-Mendoza M. et al. [39]. The chemical reagents used for
the chemical bath preparation were ZnSO4 as a source of Zn2+ ions,
KOH as a pH controller of the solution, and NH4NO3 as a complexing
agent. The temperature of the chemical bath was permanently set at
25 °C. The dissociation of ZnSO4 for obtaining Zn2+ ions is de­
scribed as,
2+ 2
ZnSO4(S) Znaq + SO4(aq)

The NH4NO3 and KOH compounds are dissociated to release NH4+

and OH-ions as they are described to
NH4 NO3(s) +
NH4(aq) + NO3(aq)

KOH(s) K(+aq) + OH(aq)

+
NH4(aq) + OH(aq) NH3(aq) + H2 O(I)
Fig. 9. XRD data for ZnO (a), NZO-2 as synthesized (b), NZO-2 calcined (c) (top).
Structural model of NZO-2 seen aong a-axis (bottom). Zn: gray, O:Red. Through chemical reactions, Zn2+ ions can react with formed OH-
or NH3 to form Zn(OH)n(n−2)- or Zn(NH3)n2+ ions.
trigger nano/micromorphological structure-based devices in the
Zn(2aq+) + nOH(aq) Zn (OH)(nn(aq2))
semiconductor technology [36]. The photon absorption in the UV
region ratifies the wide bandgap characteristics of ZnO and its ap­ Zn(2aq+) + nOH3(aq) Zn (NH3)2n +(aq)
plications, including energy harvesting and storage devices. J. Ungula

Fig. 10. SEM images of ZnO nanorods.

8
B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 11. TEM images of NZO-2 at different magnifications (a-c), SEM image of NZO-2 P (d).
Finally, the ZnO compound is formed by (i) the Zn(NH3)n2+ and
Zn(OH)n2+ ions reacting with OH to form solid ZnO, and (ii) the Zn
(OH)n(n−2)-dissociates reacting with OH to form solid ZnO.
Zn (NH3)2n +(aq) + 2OH(aq) ZnO(s) + nNH3(aq) + H 2O(I)
Zn (OH)(nn(aq2)) ZnO(s) + H 2O(I) + (n 2) OH(aq)
Fig. 12 shows considerable higher intensities of the (101) peak of
ZnO and (311) peak of Zn(OH)2. In Fig. 12b, the intensities of the (111)
peak of Zn(OH)2 and (100) peak of ZnO increase, meanwhile the
(002) peak of ZnO is now evidenced. For samples extracted at
pH= 11.40 (Fig. 12c), very sharp and high intensity of the (100), (002),
(101), and (110) peaks are notoriously observed. Finally, at pH values
slightly lower than 11.35 (Fig. 12d) the appearance of the ZnO and Zn
(OH)2 compounds is promoted again. Thus, from the presented re­
sults, it can be concluded that growing of specific compounds is
strongly determined by the precise control of the pH in the solution,
being pH= 11.40 the most adequate value for the preferential ZnO
formation at room temperature [39].
The scanning electron microscope images illustrated that the
ZNRs morphologies improved, their lengths and diameters increased
as the growth Cs and II/VI molar ratios were raised. The GZO
transparent conductive film, with good crystallization produced at
the precursor solution concentration ratio in the vicinity of 1, and a
deposition time of 18 min, can be used as a possible photoanode for
dye-sensitized solar cells. M. N. Rezaie et al. [40] employed the most
efficient and least hazardous solution-based techniques, which are
widely used for growing ZnO nanorods. The average grain size and
9
Journal of Alloys and Compounds 925 (2022) 166511
roughness of the AZO and ZnO seed layers are respectively,
46–58 nm and 30–42 nm.
Paul et al. reported a comparative study on the physical and
electrical properties of n-ZnO nanowires (NWs)/p-Si and n-ZnO
NWs/p-CuO film heterojunctions [41]. The solar energy conversion
efficiency of the n-ZnO NWs/p-CuO and n-ZnO NWs/p-Si hetero­
junctions was obtained to be 3.92% and 0.008%, respectively. G.
Fiaschi et al. demonstrated a novel approach towards the shaping
and modification of ZnO nanostructures on flexible substrates [42].
The annealing process significantly modified the crystalline struc­
ture, both in the bulk and at the surface. A new nanostructured
surface with desirable luminescence properties could be fabricated
for the development of flexible sensors and wearable bio-elec­
tronics.
The growth process of the nanostructured CdO films is re­
presented by M. Thambidurai et al. [43]. The aqueous solution of
cadmium nitrate tetrahydrate [Cd(NO3)2.2 H2O] and hexamethyle­
netetramine [(CH2)6N4], as well as the following chemical reactions:
C6 H12 N4 + 6H2 O 4NH3 + 6HCHO
NH3 + H2 O OH + NH4+
Cd2 + + 2OH Cd (OH)2
When hexamethylenetetramine is hydrolyzed with heat, it pro­
duces ammonia (NH3) and formaldehyde (HCHO). The ammonia
reacts with water, producing hydroxyl (OH-) ions. Cadmium nitrate
tetrahydrate reacts with water, forming cadmium (Cd2+) ions.
Cadmium hydroxide Cd(OH)2 is formed when hydroxyl (OH-) ions
B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 12. XRD patterns of samples deposited in the Zn(O, OH) region, a) pH= 11.60, b) pH= 11.50, c) pH= 11.40 and d) pH= 11.35.
combine with cadmium ions remove the hydroxide phase, the cad­
mium hydroxide films were annealed at 500 °C for 1 h.
Cd (OH)2 CdO + H2 O
Finally, the formed CdO nuclei tend to grow as spindle-shaped
nanostructures with an increase in molar concentration, but further
increasing concentration results in the formation of coconut fibre
bark-like CdO nanostructures. CdO films were grown by a two-step
chemical bath deposition method with the effect of molar con­
centrations. The formation of nanoparticles, spindles, and coconut
fibre bark shape nanostructures was observed under a field emission
scanning electron microscope. X-ray diffraction patterns of CdO films
with various molar concentrations are shown in Fig. 13. Three peaks
appear at (111), (200) and (220) were indexed to the cubic phase of
CdO (JCPDS Card No.: 05–0640). The absence of other impurity peaks
suggested the formation of highly pure CdO nanostructures. The
lattice constant (a) has been calculated and is found to be a = 4.70 Å.
The increase of peak intensities with molar concentration implies
the crystallinity improvement when we increased the molar con­
centration. The FESEM images of CdO films (Fig. 14a-h) grown by
chemical bath deposition with 0.01 M concentration clearly show
that grains are agglomerated. Fig. 14 (c,d) reveals the morphology of
CdO films prepared with 0.03 M concentration. We can see that the
grains start to form spindle-shaped nanostructures due to Ostwald
ripening [16] and furthermore the formation of nanospindle-like
CdO structures is confirmed in the FESEM images of CdO synthesized
using 0.05 M concentration (Fig. 14(e, f)). With increase in molar
concentration, the spindle-shaped nanostructures start to self-as­
semble in to coconut fiber bark shaped nanostructures as observed
for the CdO films grown with 0.07 M concentration (Fig. 14(g, h)).
CdO, with a typical bandgap of 2.2 eV, is one of the most important
10
Journal of Alloys and Compounds 925 (2022) 166511
semiconductors for potential applications in solar cells, photo­
detectors, and gas sensors.
3.2. Spray pyrolysis method
J.K. Saha et al. [43] fabricated metal oxide thin film transistors by
spray pyrolysis are of increasing interest because of their simple
process and scalability. The ZnO thin films were deposited on glass
by spray pyrolysis using precursor solutions without and with AA.
Fig. 15 shows the schematic diagram of the spray system. The de­
position temperature was varied from 200 to 400 °C, the flow rate
(3 ml/min) and the nozzle speed (8 cm/sec) were kept constant to
find the optimum temperature. The ZnO precursor solutions without
and with AA were sprayed from low temperatures (200 °C) to high
temperatures (400 °C). Fig. 15 (c-h) shows the optical microscopy
and SEM images of ZnO films without AA deposited on glass at 250,
350, and 400 °C, respectively. As the temperature increases, the
density and the size of the coffee rings/bubbles decrease. As shown
by SEM in Fig. 15(f-h), the films formed at 250 °C exhibit a mixture of
large rods and islands, at 350 oC only islands are formed with an
apparent decrease of the overall roughness. The rods might form due
to the limited diffusion length at low temperatures, resulting in
substrate plane nucleation and growth. At temperatures over 300 °C,
the diffusion length becomes high enough for lateral growth.
Fig. 15(i–n) shows the optical and SEM images of ZnO films de­
posited from the precursor solution containing AA at the substrate
temperature from 250 °C to 400 °C. At 250 °C, the density of bubbles
is much lower than that one in the film sprayed without AA.
Moreover, at ≥ 350 C the films do not show any bubble. The SEM
images in Fig. 15(i–n) show that films with AA consist of small is­
lands and no rods are found. The inhomogeneous nucleation at the
B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 13. (a) X-ray diffraction patterns of CdO films with various molar concentrations.
coffee ring boundaries would be due to the direct impingement of
droplets. The diameter of one ring is around 20 µm and that its
boundary is decorated with large rods. As the solvent evaporates, the
solutes are gathering at the boundary and vertical growth is dom­
inating during nucleation. The presence of AA at high substrate
temperature increases the diffusion length and slow evaporation
makes the film uniform and compact. We can see the effect of
temperature and AA on the morphology of the ZnO film. Additional
optical and SEM images for films grown at 200 °C and 400 °C. This
suggests that adding AA to the precursor solution increases the
diffusion length of the Zn precursors on the growing surface during
spray coating. The device with AA exhibits high field effect mobility
of 41.53 cm2V−1S−1, which represents an 8-fold improvement com­
pared to the TFT made without AA. This work contributes to the
development of low operating voltage, high mobility ZnO TFT with
excellent stability for the next generation of low-cost displays. The
spray deposition of zinc oxide (ZnO) thin films has been carried out
by [44–67]. The optical transmission leads to 90% in the visible re­
gion, and the optical band gap is varied from 3.22 to 3.28 eV and the
electrical resistivity is found between 1.42 Ω-cm and 17.60 Ω-cm
[45]. The surface roughness of ZnO films increased from 8.8 nm to
42.2 nm [46].
The film formation mechanism is described by A. Ani et al. [47].
The chemical reactions for the formation of ZnO from zinc acetate
dehydrate through thermal decomposition are represented in the
following equation.
400oC
Zn (CH3 COO).2H2 O Zn (CH3 COO)2 + 2H2 O
11
Journal of Alloys and Compounds 925 (2022) 166511
400oC
4Zn (CH3 COO)2 + H2 O Zn4 O (CH3 COO)6 + 2CH3 COOH
400oC
Zn4 O (CH3 COO)6 + 3H2 O 4ZnO + 6CH3 COOH
400oC
Zn4 O (CH3 COO)6 + H2 O 4ZnO + 3CH3 COCH3 + 3CO2
The ZnO film irradiated at 5 kGy exhibited enhanced response
and recovery time as well as effective response in the CO con­
centration range of 2–5 ppm at an optimized operating temperature
of 300 °C [47]. The effect of Ag doping on the morphological and
photoelectrochemical properties of ZnO thin films is synthesized by
[48]. The photocurrent density produced by the ZnO:2% Ag electrode
reached 0.44 mA/cm−2, which is about six times higher than that
measured on pure ZnO.
The sensing properties of Er-doped ZnO films were analyzed with
respect to ammonia concentrations from 25 ppm to 125 ppm as re­
ported by K.D. Arun Kumar et al. [49]. The 3% Er-doped ZnO, which
exhibits good emission behavior, could be suitable for luminescence,
detector, and sensor applications. Undoped, Al-doped, and Sn-Al co-
doped ZnO thin films have been successfully synthesized by K.Salim
et al. [50]. The electrical conductivity has increased with the Al-Sn
co-doping concentration to reach a value of 0.335 (Ω.cm)−1. Al-doped
ZnO thin films, with their high Seebeck coefficients and low
bandgap, can be used for thermoelectric and optoelectronic device
applications in their prepared state [51]. The V-doped ZnO (10%) film
exhibits a tiny but clear ferromagnetic response at room tempera­
ture, which makes this material interesting for further study of
combined semiconducting and magnetic properties [52].
Un-doped ZnO films have a hexagonal wurtzite crystal structure
with a major diffraction peak along the (002) plane and minor peaks
in the (101) and (103) planes [53–64]. With a band gap energy of
3.2 eV, ZnO is extremely useful in optoelectronics, solar cells, gas
sensors, and TFTs. The properties of nanostructured ZnO thin films
have been studied by D. Acosta et al. [65]. Un-doped and Al-doped
ZnO films have been successfully deposited by the spray pyrolysis
method and their structural, optical, and gas sensing properties have
been investigated by R.K. Shukla et al. [66]. The maximum sensitivity
at 400 °C is for higher concentrations of CO2, whereas aluminium-
doped samples show a maximum either at 350 °C or below for all
CO2 concentrations. The Fe doped ZnO films with various levels of
doping (0,1,5 & 10 at%) have been prepared by spray and the effects
of Fe doping properties on ZnO films have been studied by S. Umar
et al. [67]. W. Sripianem et al. [68] reported on Al-doped ZnO films
deposited at 400 oC with Al doping contents of 1,2,3,4, and 5 at
%.-doped films exhibited the highest sheet resistance, while the 2%
Al-doped ZnO exhibited the minimum sheet resistance.
CdO is a II-VI n-type semiconductor having a bandgap energy of
2.2 eV at room temperature and shows good electrical conductivity
and optical transparency in the visible and infrared regions [68]. B.K.
Balachandar et al. reported that pure and Al-doped CdO thin films
were coated using a facile chemical spray pyrolysis technique [68].
According to sensor studies, 1.5 wt% Al doped CdO film has a max­
imum sensitivity of 32% for trimethylamine vapour compared to
benzene, ammonia, and dimethylamine. In XRD analysis, all the
diffraction peaks strongly exhibit polycrystalline nature with a per­
fect cubic structure, followed by preferential orientation changing
from the (111) plane to the (200) plane [69]. CdO is a well-known
semiconducting metal oxide having good electrical conductivity
[70]. The possible reaction mechanism for the formation of CdO thin
films is described by P.D. More et al. [71].
Cd (CH3 COO)2 + 3H2 O ZnO + CH4 + 4H2 + 3CO2
The highest LPG response was recorded as 20% for a 10 vol% gas
concentration with fast response and recovery times of 18 s and 32 s,
respectively, at room temperature. CdO thin films can be the po­
tential material for room temperature operated LPG sensors with
B. Amudhavalli, R. Mariappan and M. Prasath Journal of Alloys and Compounds 925 (2022) 166511

Fig. 14. FESEM images of CdO films at two different magnifications. (a, b) 0.01 M, (c, d) 0.03 M, (e, f) 0.05 M and (g, h) 0.07 M.

good selectivity and stability [72–74]. The thin film formation on the reveals high mobility value when low free carrier absorbance is
heated glass substrate to pure CdO and Y:CdO films is as described described [75–77]. M. Ravikumar et al. developed a novel and simple
by S. Ahmed et al. [74]. spray technique for depositing cadmium oxide (CdO) with different
300oC
concentrations (0, 1, 3, and 5 wt%) of Eu doping onto Si glass sub­
Cd (CH3 COO)2.2H2 O + H2 O CdO + +CO2 + CH4 + steam strates [78]. Current voltage measurements on the fabricated na­
nostructured Al/Eu-nCdO/p-Si/Al heterojunction device showed
300oC
Y (CH3 COO)2.4H2 O + Cd (CH3 COO)2.3H2 O + H2 O Y non-linear electric characteristics, indicating diode like behavior.
The un-doped and F-doped CdO thin films were fabricated by M.
: CdO + +CO2 + CH4 + steam
Anitha et al. [79]. XRD spectrum of the CdO thin films deposited at
Cadmium oxide (CdO) is one of the common n-type transparent 200 °C as a function of carrier gas pressures as shown in Fig. 16. A
conducting oxide materials with a narrow bandgap of 2.4 eV and strong intense peak is obtained at 2θ = 33.05° for CdO thin films,

12
B. Amudhavalli, R. Mariappan and M. Prasath Journal of Alloys and Compounds 925 (2022) 166511

Fig. 15. Nucleation and surface morphology of ZnO thin film without and with ammonium acetate (AA) deposited by spray pyrolysis at substrate temperature of 250, 350, and
400 °C. Schematic of (a) the spray system used for the experiment and (b) the nucleation process at the time of pyrolysis. Optical microscopy and SEM image of ZnO thin films
deposited at 250, 350, and 400 °C (c–h) without and (i–n) with AA in precursor solution. After direct impingement of droplet on the hot substrate, the droplet changes the phase
from vapor to solid and results unwanted coffee rings. The presence of AA in precursor solution helps the droplet to levitate on the substrate and increase the diffusion length on
the substrate. As a result, coffee rings free uniform film with high compactness are found by slow evaporation of solvents.

CdO thin films as a function of different carrier gas pressure is shown

Fig. 16. XRD patterns of CdO thin films as a function of different carrier gas pressure.
which indicates a preferential orientation along the (111) plane with
cubic structure (Fm3m space group) and all the diffraction peaks­
were indexed by matching JCPDS data (card no 05–0640). The dif­
fraction peak intensity of the CdO thin films had increased as the
carrier gas pressure had increased and gets sharper with decreased
in full width at half-maximum from P1 to P3 and then the intensity
decreased for higher carrier gas pressure. The surface morphology of
in Fig. 17. The microstructure of all the thin films is homogeneous
and uniformly distributed sphere like grains throughout the surface.
The thin film deposited with P1 carrier gas pressure is seen to have
irregular sphere like structure with small pin holes. It has been
observed that sphere like CdO grains are found to be increase in size
with an increase in carrier gas pressure up to P3 and then decreased
in grain size for higher carrier gas pressure The CdO thin film coated
with P5 carrier gas pressure the surface appears to be non-sphere
like structure because the particle vulnerable against the high carrier
gas pressure due to the evaporation of the trapped liquid in the
particle. The high carrier gas pressure can also cause particle colli­
sions, which result is further particle disruption. Thus the SEM re­
sults corroborate the X-ray results that the particles peak intensity
and crystallite size increases when carrier gas pressure increases.
The attained sphere like grains may provide better implementation
for solar cell applications. The minimum resistivity value of 1.9 × 10−4
Ω-cm with notable higher values of carrier concentration and mo­
bility was achieved for 6 at% of the CdO:F film. The tin-doped cad­
mium oxide (Sn: CdO) transparent thin films with different Sn
concentrations were deposited on glass and p-silicon substrates by
the chemical spray method at 250 °C [80]. The optimal level of Sn in
CdO could improve the CdO properties, and it can be used for the
fabrication of heterojunction photodiodes. For 14.7 × 104 (Nm−2)
carrier gas pressure of CdO thin film, high carrier concentration
(2.88 ×1019 cm−3), low resistivity (4.76 ×10−3 Ω-cm), and a high figure
of merit (25.0 ×10−3) were observed [81].
The CdZnO films are very useful for the fabrication of ZnO/ZnCdO
heterojunction and superlattice structures, which are the key ele­
ments in ZnO-based light emitters and detectors [82,83]. Recent
development of low cost nebulizer sprayed Cd1−xZnxO nanoparticles
are reported by B. Amudhavalli et al. [83]. X-ray diffraction patterns

13
B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 17. SEM images of CdO thin films as a function of different carrier gas pressure.
recorded for Cd1−xZnxO thin films are deposited at different con­
centrations (x) with substrate temperature 400 ◦C as shown in
Fig. 18a-g. The different peaks in the diffractogram were indexed and
the corresponding values of the interplanar spacing ‘d′ were calcu­
lated and compared with the standard values. For x = 0, the crystal
structure of CdO thin films is the cubic crystal structure, which is
similar to that of X-ray diffraction peaks corresponding to (111),
(200), (220), (311) and (222) planes with compared JCPDS No.
05–0640. For x = 1.0, however, ZnO films were grown with hexagonal
structure with the prominent X-ray diffraction peaks corresponding
to (100), (002), (101), (102), (110), (103) and (112) planes with
compared JCPDS No. 36–1451. For x ≥ 0.1 to x ≤ 0.9, however, the
Cd1−xZnxO films exhibit mixed phases of the cubic and hexagonal
crystal structure with preferential orientation along (111) and (002)
14
Journal of Alloys and Compounds 925 (2022) 166511
planes. It is clearly that the intensity of the peak (111) decreased
with increased Zn content. Fig. 19a-e shows the high resolution
scanning electron micrographs of Cd1−xZnxO films grown at con­
centrations x = 0, 0.25, 0.50, 0.75 and 1, respectively. It is seen from
Fig. 19a-e, the surface morphology and grain size changed with the
increase concentration (x). As the concentration x = 0, the clusters
formed from the nanostructured particle are shown is Fig. 19a.
Further increased concentration x = 0.25, 0.5 the granular surface of
Cd0.75Zn0.25O, Cd0.5Zn0.5O film belonging to the transition between
tow structures has mixed together as observed in Fig. 19b and c. As
the concentration increased to x = 0.75 (Fig. 19d), small with uniform
spherical grains and well-defined grain boundaries with average
grain were found to be ~34 nm. It can be seen from Fig. 19e (x = 1.0),
the smooth, dense, uniform platelet-like structures and porous space
B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 18. XRD patterns of Cd1-xZnxO thin films:(a) x = 0, (b) x = 0.25, (c) x = 0.4, (d)
x = 0.5, (e) x = 0.75, (f) x = 0.9 and (g) x = 1.0.
with average grain size is ~55 nm. The CdZnO fim prepared from
aged solution possesses a high crystallite size value of 38.72 nm and
low strain and dislocation density values of 0.89 × 10−3 and
0.667 × 1015 lines/m2, which supports its enhanced crystallinity. T.
Noorunisha et al. [84] have presented nanostructured ternary CdZnO
thin films with zinc concentrations of 0, 2, 4, 6, and 8 wt% that were
prepared by the spray pyrolysis technique using a perfume atomizer
on glass substrates at 375 °C. The optical band is red-shifted with an
increase in annealing temperature, which can be related to quantum
confinement. CdxZn1−xO (0 ≤ x ≤ 0.20) thin films with different Cd
concentrations were successfully deposited on glass substrates using
the spray pyrolysis technique [84]. The CdxZn1−xO thin films with a
10% cadmium concentration showed a sensitivity of 50% for 1 ppm
ethanol.
3.3. Sol-Gel spin coating method
ZnO-based materials are getting a lot of research due to their
potential applications in electronic, optoelectronic, and sensing de­
vices, as well as ultraviolet light-emitting and laser diodes [85–90].
Zinc oxide is one of the most widely studied semiconductor metal
oxides, which predominantly crystallizes as hexagonal wurtzite and
often cubic zinc-blende phases. Sauvik Chatterjee et al. [91,92] have
report the transformation of the highly stable wurtzite ZnO to a new
triclinic phase NZO-2 by using metformin as a template during post-
synthesis hydrothermal treatment. This crystalline phase of the
material NZO-2 has been identified through the refinement of the
powder XRD data. The powder XRD of NZO-2 was recorded to
identify the crystalline phase and its unit cell parameters. As seen
from Fig. 20 top, NZO-2 displayed a new crystalline phase with sharp
peaks at 9.44, 13.46, 16.40, 19.23, 20.54, 21.41, 27.03, 28.81, 30.34,
31.86, 33.17, 34.47, 40.77 and 41.42 degrees of 2θ for both the as-
15
Journal of Alloys and Compounds 925 (2022) 166511
synthesized and calcined samples. These peaks could be assigned to
the triclinic phase of NZO-2 with P1 space group. The unit cell
parameters of this phase is: a= 9.605, b= 8.083, c= 6.107 Å, α = 104.58,
β = 97.66° γ = 98.94°. The unit cell volume for this phase was found to
be 446.2 Å. Although it is evident from the PXRD pattern of as syn­
thesized NZO-2 that the formation of the triclinic phase occurs
during the hydrothermal synthesis, the crystallinity of the newly
formed triclinic phase is quite high and it has been improved con­
siderably after calcinations. NZO-2 possesses porous rod like particle
morphology consisting of the self-assembly of 3–7 nm size spherical
nanoparticles and interparticle nanoscopic voids spaces. M.E.I.
Ahmed et al. [93] have developed ZnO thin films deposited by the
sol-gel technique and films that have a hexagonal wurtzite structure
with a crystallite size of 48 nm. D. Ali et al. have successfully syn­
thesized La and Sm doped ZnO thin films on Si substrate using the
sol-gel spin coating method. Better photodegradation of methylene
blue has been obtained for La and Sm doped ZnO films [94]. Based on
un-doped and (Ce,Al) co-doped ZnO films, Schottky diodes have
been fabricated by M.A.M. Ahmed et al. [95]. Fig. 20 shows the X-ray
diffraction (XPERT-PRO diffractometer, PAN analytical BV, Nether­
lands) patterns of ZnO thin films deposited onto ITO/glass substrate.
In the XRD patterns, there are strong peaks corresponding to the
(100), (002) and (101) planes. Small peaks corresponding to the
(102) and (110) planes were also observed, indicating that the films
have hexagonal wurtzite structure. It is clear from this pattern that
the films consist of randomly orientated polycrystalline particles
with a slightly preferred orientation along (002) plane. The values of
the lattice constants obtained are in good agreement with the values
from the JCPDS data with card number (76–0704). Fig. 21 shows the
SEM image of ZnO thin films annealed at different temperatures. The
SEM image shows a uniform compact surface. The surface mor­
phology of the samples was represented by different ganglia-like
hills with typical width of about 1 µm and a height of 5–10 µm. The
surface of the thin film, annealed at 300 °C, contained some cracks
while no crack was observed after annealing at 400 °C, and 500 °C.
The highest density thin film was achieved after annealing at 500 °C.
As the annealing temperature of ZnO films increased from 300 °C to
500 °C, the volume and size of ganglia-like hills increased and the
films became denser. The I-V characteristics of fabricated Schottky
diodes manifest good device behaviour at higher levels of doping
(7.0 at%) with an ideality factor of 2.40, a barrier height of 0.77 eV,
and series resistance of 262 Ω.
Mirkhani et al. have fabricated a set of bottom-gate ZnO thin film
transistors (TFTs) with active layers containing 1, 4 and 8 layers of
spin-coated ZnO [96]. Zinc oxide semiconductors belong to trans­
parent conducting oxides (TCOs). This oxide is characterized by high
transparency in the visible range, a wide optical band gap of 3.37 eV,
a large exciton binding energy of 60 meV at ambient temperature,
electrical conductivity, and thermal stability [97–99]. S. H. Sabeeh
et al.[100] describe the chemical reactions of ZnO thin films.
Zn (CH2 COO)2 .2H2 O + 2(NH2 CH2 CH2 OH) 2H2
O + CH3 CONHCH2 CH2 OH2 + Zn (OH)2
Zn (OH)2 ZnO + H2 O
The ZnO thin film sensor was developed using a low-cost sol-gel
spin coating technique on a glass substrate [101–105]. Moreover, the
ZnO thin film sensor shows a fast response and recovery time of 2 s
and 137 s, respectively, upon 100 ppm NO2 exposure with excellent
stability (68%) and repeatability. The response and recovery times of
the ZnO sensor were found to be quite fast for NO2 as compared to
other gases (NH3, CH3OH, Cl2, and H2S) [105].
Undoped and Cd-doped ZnO (Cd:2, 5, and 10 wt%) semiconductor
thin films were prepared by the sol-gel route technique as described
by B. Rahal et al. [106]. The optical gap decreases from 3.21 to
B. Amudhavalli, R. Mariappan and M. Prasath Journal of Alloys and Compounds 925 (2022) 166511

Fig. 19. HRSEM images of Cd1-xZnxO thin films: (a) x = 0, (b) x = 0.25, (c) x = 0.5, (d) x = 0.75 and (e) x = 1.0.

3.08 eV as the doping increases, and this is confirmed by the pho­

Fig. 20. The X-ray diffraction (XRD) patterns of ZnO thin films deposited onto ITO/
glass substrate after annealing at 600 °C.
toluminescence spectra of films, which also show the emissions in
the ultraviolet (UV) and visible [106]. AFM analysis revealed the
uniform nanowire growth of MZO films where each nanowire was
made up of very fine nanoparticles. The grain size was found to be
increased from 16 to 25 nm with increasing Mg-doping, which
agreed with the crystallite sizes obtained from the XRD analysis
[107]. TM-doped ZnO has been considered one of the most pro­
mising diluted magnetic semiconductor (DMS) materials. Also, the
optical properties, such as complex dielectric function, refractive
index, optical reflectivity, absorption coefficient, energy-loss spec­
trum, and complex conductivity function, were found to be shifted
toward the lower energy of incident photons as the Mn concentra­
tion increased [108,109].
Under hydrolysis conditions, the cadmium acetate dehydrate is
used as a precursor salt. The cadmium acetate molecule gives the ion
Cd2+. The possible initial reaction steps are as follows [110].
Cd (CH3 COO)2 Cd2 + + C (CH3 COO)
Cd2 + + 2(H2 O) + 2OH Cd (OH)2 + + 2H2 O

16
B. Amudhavalli, R. Mariappan and M. Prasath Journal of Alloys and Compounds 925 (2022) 166511

Fig. 21. SEM image of the ZnO thin films at different annealing temperature (A) 300 °C (B) 400 °C (C) 500 °C.

Thus, Cd (OH)24 a complex is formed. This assumes the function of

nucleating units to create CdO nano-structures.
Ganesh et al., have discussed the CdO/FTO films with a different
doping concentration that are prepared by a sol-gel spin coating
technique. The dielectric constant (ε1), loss (ε2), refractive (n) and
absorption (k) indices, linear (χ(1)) and nonlinear (χ(3)) suscept­
ibilities and nonlinear refractive index (n(2)) values were also esti­
mated [110]. CdO films with various solution molarities were
deposited on the SLG substrates by the sol–gel spin coating method.
The optical band gap decreased with increasing molarity, showing
agreement with literature results [111]. Transparent conductive
oxides (TCOs) have emerging applications in optoelectronic tech­
nology as described by S. AlFaify et al. [112]. XRD analysis was per­
formed to investigate the crystal phase in the CdO thin films. Fig. 22
displayed all the diffraction peaks of the M1, M2 and M3 films and
the patterns are well consistent with the JCPDS card no. 05–0640.
Intense peaks are observed at 2θ values of 33.54°, 38.76° and 55.65°
corresponding to the (111), (200) and (220) crystal planes, respec­
tively indicating the successful formation of the CdO phase with a
face-centered cubic structure (Space group Fm3m). The intensity of
the (111) peaks is a maximum for the M1 sample as compared to the
other samples. A slight shift to a higher angle in the peak position
was observed for sample M1 and M3, which may be related to the
Fig. 22. XRD patterns of CdO thin film of different molar concentration with JCPDS molarity of the solution. At the low molarity (0.2 M) the M1 film was
card no 05–0640.
not deposited uniformly as clearly seen below in the SEM results.
Therefor more strain is produced and some shifting with respect to
The cadmium hydroxide Cd(OH)2 dissolves in the solution as the the peaks from the standard JCPDS data (JCPDS card no 05–0640)
amount of precursor salt increases, forming a complex. was observed. With the increase in the molarity of the solution more
uniformed films with peaks that match the standard JCPDS data
Cd (OH)2 + 2H2 O Cd (OH)24 + 2H+ + 2H+ were obtained. When the molarity concentration was increased

17
B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 23. SEM images of the CdO thin films (A) 0.2 M, (B) 0.5 M and (C) 0.8 M.
further two phases were formed and a double peak for M3 was
observed. The two phases may be due to different layers that formed
near the substrate and the top layer of the films. The layer near the
substrate might contain some glass elements (Na ions) with the CdO
and represented as in M1 while the top layer consisted of pure CdO
so the double peak for the M3 sample was obtained due to the
mixing of the two phases (M1 & M2). This suggests that the 0.5 M
thin film was uniform and well matched with the cubic crystal of the
CdO. It must, however, also pointed out that with the thicker layers
formed at the higher molarity that less strain might occur in some
parts of the films with other parts still containing some strain that
will also led to a broadening and shifting of the peaks leading to the
double peaks. In Fig. 23, the SEM micrographs clearly show that the
precursor concentration of the CdO affect the surface morphology of
the films. Fig. 23(a) shows the SEM image of the M1 film revealing
the typical morphology of albumen that was spread non-uniformly
due to the lower molarity concentration and indicating particle ag­
glomeration with small grains. Fig. 23(b) shows a cauliflower like
surface morphology of the M2 film. The SEM image shows a closely
packed arrangement of the crystallites. Fig. 23(c) shows the SEM
image for the M3 sample. The surface of the thin films was rough
and the albumen formed clusters in an irregular way. The surface
morphology of the M3 thin film shows cubic like clusters which is
also promoting the cubic structure of the CdO. Surface morphology
of M3 films show that it contains two or more layer that generate
different phase which is identified by XRD result as mix phase is
obtained. Hence, we have designed and fabricated the cadmium
oxide (CdO/FTO) TCO films with different concentrations of
18
Journal of Alloys and Compounds 925 (2022) 166511
lanthanum (La) through a facile spin coating technique. The average
values of grain size were estimated in the range of 7.56–10.95 nm,
along with surface roughness in the range of 15.25–17.56 for pure
and La-doped CdO films. The optical band gap value of undoped-CdO
continually declines, but the Urbach energy values increase with Si-
doping levels [113]. The electrical resistance of the 0.5 M thin film
was found to be 1.56 k. In the low temperature range (32–200 °C),
the oxygen sensing response was found to be between 20% and
33% [114].
CdZnO thin films with different ratios of CdO and ZnO (3:1, 1:1,
and 1:3) were grown on glass substrates using the sol–gel spin
coating method as reported by R.K. Gupta et al. [115]. The surface
morphology of various films was studied using atomic force micro­
scopy. The AFM images of pure ZnO, CdO, and CdZnO films are
shown in Fig. 24. All the images were taken in 40 µm x 40 µm area.
As observed in Fig. 24, pure ZnO and CdO films are different in
morphology. ZnO film shows fiber structure, while CdO film shows
grain like structure with grain size of few nanometers. On the other
hand, the morphology of CdZnO films depends on the percentage
compositions of ZnO and CdO. Films having higher amount of CdO
shows the presence of grains along with the fiber nature of ZnO,
whereas, the film with lower percentage of CdO shows fiber nature
of the film very similar to pure ZnO film. The effect of copper doping
on the surface morphology of ZnO films was reported. It was ob­
served that the surface characteristics of all samples were same, only
the roughness and crystallite size were changing with copper
doping. The optical bandgap of CdZnO (3:1), CdZnO (1:1), and CdZnO
(1:3) films was calculated to be 2.80, 2.49, and 2.52 eV. The chemical
B. Amudhavalli, R. Mariappan and M. Prasath Journal of Alloys and Compounds 925 (2022) 166511

Fig. 24. AFM images of (a) ZnO, (b) CdO, (c) CdZnO (3:1), (d) CdZnO (1:1), and (e) CdZnO (1:3) films (the area of all images is 40 lm _ 40 lm).

states and the composition of the surface of sol-gel derived CdZnO temperatures as normally displayed by ZnO films. The green-yellow
thin films were studied by X-ray photoelectron spectroscopy (XPS) luminescence associated with these defects was observed at higher
[116,117]. The transmission and band gap decreased with an increase annealing temperatures (700° C).
in Cd content [116]. As composition and structure changed due to the
Cd volume ratio, the order of the carrier concentration was varied 3.4. Electrodeposition coating method
from 1016 to 1020 cm−3 with the Cd ratio and the mobility increased
from less than 2–45 cm2 V−1s−1. [118]. A. Singh et al. [119] have The mechanism of the electrochemical deposition of ZnO films
fabricated ternary ZnCdO thin films oriented along the c-axis that can be described as follows [120].
have been successfully deposited on p-Si (100) substrates using the
NO3 + H2 O + 2e NO2 + 2OH
sol-gel spin coating route. Room temperature did not exhibit any
luminescence related to oxygen vacancy defects for lower annealing
Zn2 + + 2OH Zn (OH)2

19
B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 25. SEM images of ZnO/ITO system before and after the polarization test with UV illumination in Fig. 6, (a) before, (b) after.
Zn (OH)2 ZnO + H2 O
The side reaction of hydrogen evolution would occur at more
negative potentials:
2H+ + 2e H2
As described by the above equation, NO3-will be converted into
NO2-near the cathode, and then the pH near the cathode will rise,
leading to the reaction of Zn2+ with OH to form Zn(OH)2 on the
cathode surface (Equation 2). Finally, Zn(OH)2 will be dehydrated
and converted to ZnO at a temperature above 34 °C.
The possible anodic and cathodic reactions that occur on the
ZnO/ITO electrode system at undisturbed or polarised states may be
written as follows:
4OH 2H2 O + O2 = 4e (Anodic)
2H2 O + O2 + 4e 4OH (Cathodic)
2H+ + 2e H2 (Cathodic)
The UV illumination leads to a significant increase in the anodic
current density for the ZnO/ITO system. The enhanced current
density may come from an additional anodic reaction due to the
photo-generated holes. Under UV illumination, electron-hole pairs
are generated within the ZnO nanorods.
h The possible formation mechanism of CdO is suggested as fol­
ZnO ZnO + h+ + e
The photo-induced electron could transfer to the SS304, resulting
in a negative shift in potential.The holes remain in the valence band
of ZnO, oxidising water according to the formula below.
4H+ + 2H2 O O2 + 4H+
Therefore, the anodic current density for the ZnO/ITO under UV
illumination is the sum of the anodic current densities of anodic
reactions.
Liu et al. [120] have prepared ZnO nanoparticles which were
deposited potentiostatically on the surface of stainless steel 304
(SS304) at various potentials (−0.7 V,−1.0 V,−1.3 V, −1.6 V) to study
the effect of photo-generated cathodic protection on the substrate.
Fig. 25 shows the morphology of the ZnO nanorods on the ITO
substrate before and after the potentiodynamic polarization tests
under UV illumination. It can be seen that the polarization test did
not lead to any change in the distribution and morphological char­
acteristics of the ZnO nanorods. The results confirm that ZnO might
act as a non-sacrificial anode material in photocathodic protection.
Ga-doped zinc oxide (GZO) branched nanoparticles are synthesised
by sol-electrophoretic deposition to investigate structural, morpho­
logical, size distribution, and optical properties evolution induced by
Ga content. This was investigated by A.M. Hallajzadeh et al. [121]. Ga
dopant in a concentration of 1 mol% of Ga/Ga+Zn shows the most
proper morphological and structural results. In order to improve the
20
Journal of Alloys and Compounds 925 (2022) 166511
efficiency of solar cells, various techniques considering different
aspects have been employed [122–126].
Improved photovoltaic performance of perovskite solar cells is
demonstrated through the synergistic effect of electrodeposited ZnO
nanorods and rubrene: As electron and hole-transporting layers,
they are employed by C.M. Pelicano et al. [127]. A perovskite solar
cell optimized with ZnO nanorods and rubrene: P3HT bilayer
achieved a maximum efficiency of 4.9%, showing reduced hysteresis
behaviour compared with the device having P3HT as the only hole-
transporting layer. The performance of the Cu2O/ZnO heterojunction
solar cells with different Cu2O absorber thicknesses exhibited the
highest power conversion efficiency of 0.52%. [128]. Various
morphologies of ZnO, including rods, disks, and nanosheet networks,
were synthesized by Gromyko et al. [129]. The formation of the disk-
like ZnO structure with a diameter of ca. 300–500 nm and a thick­
ness of ca. 80–100 nm was observed when 0.03 mmol/L of SeO2 was
added to the solution. Nanostructured zinc oxide (ZnO) thin films
were synthesized via an electrodeposition and subsequent heat
treatment method. The films develop a variety of microstructures
with distinct properties and characteristics when annealed at tem­
peratures ranging from 300 °C to 600 °C. The ZnO film fabricated at
500 °C has a relatively high surface area and the strongest photo­
catalytic activity, which is relatively stable after subsequent reaction
cycles [130–132].
lows, as described by A.Kiyak Yildirum et al. [133].
NO3 + H2 O + 2e NO2 + 2OH
Cd2 + + 2OH Cd (OH)2
Above 280 °C, the following reactions occur to convert Cd(OH)2
to CdO:
Cd (OH)2 CdO + H2 O
Thin films of CdO were deposited by an electrodeposition tech­
nique onto ITO-coated glass substrates. Yildirum et al. [133] used
various concentrations of Cd(NO3)2 aqueous solutions, such as 0.01,
0.04, and 0.08 M, for the first time to investigate the effects of con­
centration. XRD patterns showed that good crystallisation formed at
0.01 M of concentration. The crystallite sizes of the CdO films were
calculated using the Debye-Scherrer formula. When the pH of the
solutions decreased from 8 to 5, the energy band gap also decreased
from 2.41 eV to 2.04 eV proportionally. When the band gap of the n-
type layer varies between 1.7 and 2.08 eV, it is suitable for thin film
solar cells.
Effects of pH on CdO films deposited onto ITO coated glass sub­
strates by electrodeposition are described by B. Altıokka et al., [134].
Thin films of CdO were deposited onto indium tin oxide (ITO) coated
glass substrates using electrodeposition method. The pH of the final
solutions was adjusted from 4 to 8 and effects of pH on the films
B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 26. SEM images of the CdO thin films for (a) pH = 8 (b) pH = 7 (c) pH = 6 (d) pH = 5 and (e) pH = 4.
were investigated. The maximum film thickness was reached at pH 5
and XRD studies showed that this film had relatively high peak in­
tensities. Optical studies showed that band gap varies between 2.04
and 2.41 eV and depend on pH. The surface images of the CdO thin
films synthesised at various pH values are given in Fig. 26. There are
no cracks, voids or pinholes seen on the surface of the films and
surfaces are covered well with CdO crystals. There are nearly same
morphologies in Fig. 26a-c which are surface images of the films
obtained at pH values equal to 8, 7 and 6 respectively. The surfaces
consist of polymorphic CdO crystals and under this, there is sheet-
like structure. Fig. 26d-e show the surfaces of the films obtained at
pH 5 and 4 respectively. These two surfaces resemble each other.
There are pyramidal forms of CdO crystals on these two surfaces.
Fig. 26 demonstrates that surface morphology depends on the pH
value of the solution.
3.5. Successive ionic layer adsorption and reaction (SILAR) coating
method
The chemical reaction to deposit ZnO films is given by [135].
ZnSO4 + 2NaOH Na2 ZnO2 + H2 SO4
Na2 ZnO2 + H2 O ZnO + 2NaOH
21
Journal of Alloys and Compounds 925 (2022) 166511
The ZnO nanorods electrochemically deposited on the FTO sub­
strate were covered with CdSe by means of two different proce­
dures: successive ionic layer adsorption and reaction (SILAR) and
electrochemical pulse methods. The effect of Sr doping revealed a
change in crystal orientation from the (0 0 2) to the (1 0 1). SEM
analysis reveals the formation of flower-like morphology formed by
a number of nanowires with doping concentration [135]. For the first
time, a compact ZnO layer over a large area is deposited in a one-
step synthesis approach, without any assistance from a seed layer, by
using hydrazine hydrate as a source of hydroxyl ions [136].
363K
Zn (OH)2 ZnO
The SEM images of Z60, Z120 and Z180 thin films are displayed in
Fig. 27, in which we can clearly see formation of nanorod like
structures covering almost entire substrate area. It is evident from all
SEM images of thin films that most of the nanorods were grown with
some inclination with few exceptions of perpendicular growth to the
substrate. Fig. 27a also illustrates SEM image of a thin film deposited
for 20 cycles. From SEM images we can clearly see sparse growth of
nanorod like crystals and no nucleation at many places. Surprisingly
the length of these grown nanorods was found to be up to few mi­
crometers. The plausible reason behind sparse growth is 20 cycles
are not sufficient to produce nucleation over entire substrate area.
The SEM image of Z60 depicts that some regions were not covered
B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 27. SEM images of ZnO thin films deposited for a) 20, b) 60 (Z60), c) 120 (Z120) and d) 180 (Z180) cycles.
fully as shown in red colored circle in Fig. 27b. The diameter and
coverage of the nanorods were found to be increased in Z120 thin
films than Z60 thin films. Nonetheless, few nanorods were found to
be attached to the other inclined nanorods in case of Z120 thin films
as shown in Fig. 27c with red circles. Interestingly, uncovered sub­
strate area was also found to be reduced and a network of nanorods
was observed without any overgrowth. For Z180 thin film entire
substrate was covered with nanorods forming dense network be­
tween them as seen in Fig. 27d. Incidentally, overgrowth was ob­
served on top of the c-axis oriented rods (perpendicular to the
substrate) and these rods were grown almost parallel to the sub­
strate as shown in the red circle in Fig. 27d. The nanorods which
were grown parallel to the substrate were not connected to the
substrate. In all thin filmswe found variation in the length and the
diameter of these rods. In short, with increase in numbers of SILAR
cycles more and more rods were grown and variation in their aspect
ratio and inclination was also noted.
Gas sensing device development is a key field of research in the
current scenario. Hence, in this work, facile fabrication of ZnO films
with diverse content of Ag was accomplished as a vapour sensor, as
reported by K. Radhi Devi et al. [137]. Enhanced room temperature
ammonia gas sensing properties of pure strontium doped ZnO thin
films by the cost-effective SILAR method [138–143].
The chemical reactions of ZnO films that take place during the cycle
are given below [140].ZnCl2 + 4NH4 OH [Zn (NH3)4]2 + + 4H2 O + 2Cl
[Zn (NH3)4]2 + + 4H2 O Zn2+ + 4NH4+ + 4OH
Zn2 + + 2OH Zn (OH)2
The responsivity of 5 wt% Ag-doped film was 15 times that of
undoped ZnO film. S. Syed Zahirullah et al. [144] have prepared pure
and bi-doped ZnO thin films for gas sensing applications. The
maximum response of the films at 1000 ppm of ethanol was found to
be around 60% at an operating temperature of 400 °C.
The mechanism of CdO and Zn-doped CdO thin film formation on
the glass substrate by the SILAR method can be described as follows
[145–148].
22
Journal of Alloys and Compounds 925 (2022) 166511
Cd (NO3)2 + 2NH4 OH Cd (OH2)(s) + 2NH4+ + 2NO3
When all of the grown samples were annealed at 200 °C, the
reaction can be summarised as follows:
Cd (OH2)(s) CdO (s) + H2 O
CdO and Zn-doped CdO thin films were well adherent and see­
mingly uniform. The mechanism of Cd(OH)2/CdO film formation
using the SILAR method is as follows. In the present case, the first
precursor, alkaline zinc nitrate solution, is complex with ammonia
solution to obtain a precipitate of zinc hydroxide. As a byproduct,
ammonium nitrate is also obtained. But in the presence of excess
ammonia solution, the precipitate of tetraaminezinc (II) complex is
formed, and these reactions are represented as follows [148].
Cd (NO3)2 + 2NH4 OH Cd (OH)2 + 2NH4 NO3
Cd (OH)2 + 4NH4 OH [Cd (NH3)4]2 + + 2OH + 4H2 O
[Cd (NH3)4]2 + + 2NaOH Na2 Cd (OH)4 + 4NH3
Na2 Cd (OH)4 + H2 O Cd (OH)2 + 2NaOH
450oC
Cd (OH)2 CdO + H2 O
Guney et al. [148] have been undoped and 0.3%, 1.7%, and 4.5%
Zn-doped CdO thin films were grown by the successive ionic layer
adsorption and reaction (SILAR) method on the soda lime glass
substrate at room temperature. XRD measurements of all films were
taken via Cu-Kα (1.5406 Å) in the 2θ angle between 20 and 80. Fig. 28
shows X-ray difraction patterns of CdO and Zn doped CdO thin films.
According to the standard value of ICSD standard card number
03–065–2908 the samples are the cubic structure of monteponite
CdO. It was observed that there was no change in the crystal
structures of the samples with Zn doping. By the fact that the diluted
Zn+2 ions are easily dissolved in the core of the CdO and are collected
on the crystallite and grain boundaries of the host CdO. All undoped
and Zn doped CdO nanostructures were exhibited peaks around
32.9°, 38.3°, 55.3°, 65.9° and 69.3° at 2θ angles (111), (200), (220),
B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 28. XRD pattern of undoped and Zn doped CdO thin films.
(311) and (222) planes respectively. It is also seen here that there are
no peaks of doping Zn+2 ions in the structure.
SEM measurements were taken to show how the samples were
morphologically affected by doping Zn. As seen in Fig. 29, it is ob­
served that the sample is affected seriously morphologically by the
increase of the doping Zn. It is seen that the undoped CdO nanos­
tructures are the nanosheets and this structure is a more regular
structure in the Zn doped CdO. Due to the increase in the doping
rate, these nanostructures have thickened in the structure, and it
seems that these thin structures come together side by side. It is
observed that 4.5 Zn doped CdO samples, the structure changed
entirely and cylindrical structures were formed. It is thought that the
cause of these structures is due to Zn addition. In this case, it can be
said that the contribution of Zn to morphological structures of CdO
thin films is considered influential. The Raman spectra of undoped
and Zn-doped CdO thin films were observed to be 288 cm−1,
557 cm−1, and 937 cm−1. CdO (cadmium oxide) thin films have
Fig. 29. SEM images of undoped and Zn doped CdO.
23
Journal of Alloys and Compounds 925 (2022) 166511
recently attracted considerable interest due to their many ad­
vantages, such as growth conditions, morphology, size, direct and
bandgap variation, wide permeability variation, surface roughness
control, low resistivity, and chemical stability. Potential applications
of CdO are determined by the material's physical and optical prop­
erties. As a substantial n-type semiconductor, CdO has a direct en­
ergy band gap of 2.2–2.7 eV [149–155].
Recently, the synthesis and characterization of binary and ternary
transparent conductive oxides (ZnO, CdO, CuO, ITO, CdZnO, ZnMgO,
etc.) has become a more and more active research field because of
their scientific significance and potential for various technological
applications such as light emitting diodes (LEDs), ultraviolet pho­
todetector, UV-blue lasers, flat panel displays, solar cells, and gas
sensors. The nanostructured CdxZn1−xO (x = 0, 0.25, 0.50, 0.75, 1) thin
films were synthesised on glass substrates via the Successive Ionic
Layer Adsorption and Reaction (SILAR) method, which was em­
ployed by M. Ali Yildirum et al. [156]. Fig. 30 shows the SEM mi­
crographs images of CdxZn1−xO thin films. As seen in Fig. 30, ZnO
film (x = 0) has a smooth, homogeneous surface morphology and
covers the substrate well. The uniformity, density, and smoothness
of the films have decreased with increasing Cd concentration (x).
Consequently, the surface properties of the CdxZn1−xO thin films
appear to have changed significantly with film composition. The
energy bandgap values decreased from 3.30 to 2.22 eV with Cd
concentration (x). The nanostructured CdxZn1−xO thin films were
found to be very sensitive to light.
3.6. Chemical vapor deposition method
Ding et al. [157] have presented the fabrication of ZnO thin films
containing nanosized structures and high concentrations of zinc
interstitials for NO2 and ethanol monitoring. The obtained ZnO na­
noparticulate and nanopyramidal thin films yielded an outstanding
response of 41–1 ppm NO2 and 236 towards 100 ppm ethanol. Ex­
tensive comparison with other n-type and p-type oxides reveals that
ZnO (doped with Ga and Al) is currently the bulk oxide with the
largest ZT = 0.65 at 1000 °C [158]. The substrates were baked at 350,
B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 30. SEM images of CdxZn1−xO thin films at 15000 x magnification.
400, and 450 °C using the aerosol assisted chemical vapour deposi­
tion (AACVD) technique as reported by T. Xaba et al. [159]. The op­
tical characterization of ZnO thin films deposited on the glass
substrate reveals the direct optical band gap in the range of
3.15–3.08 eV [160–162]. Atmospheric-pressure chemical vapour de­
position using ZnO films was grown on glass substrates with ion-
plated Ga-doped ZnO (GZO) buffer layers at various substrate tem­
peratures by atmospheric-pressure chemical vapour deposition
using Zn powder and water as precursors, as employed by T. Ter­
asako et al. [163].
Fig. 31 shows the XRD patterns of the GZO buffer layer and the
films grown on the GZO buffer layer at the different TSs.The XRD
pattern of the film grown at TS= 550 exhibits a dominant (002) peak
together with weak (100), (101), (112) and (004) peaks. When the TS
increases from 550° to 600°C, weak (102), (110) and (103) peaks
appear in addition to the (100), (002), (101), (112) and (004) peaks.
The films grown at TS= 700 and 775 °C exhibit a very (201) peak
other than the peaks mentioned above. Fig. 32 shows the top and
bird’s view SEM images of the ZnO/GZO films grown at the different
TSs. The film grown at TS= 550 °C is composed of the grains have
rounded shapes with the widths ranging from 60 to 140 nm. When
the TS increases from 550° to 600°C, the grain sizes are enlarged
accompanied with the changes in shapes. At TS= 600 °C, the grains
have polyhedral shapes and their widths are distributed in the range
24
Journal of Alloys and Compounds 925 (2022) 166511
from 160 to 780 nm. Further increase in TS leads to a dramatical
change in surface morphology. The film grown at TS= 700 °C exhibits
sharp rock- like three dimensional structures on the terrace- like
surface. The appearance of the terrace- like morphology implies the
enhancement of the two-dimensional lateral growth. Although the
terrace-like surface similar to this are also observed on the films
grown at TS= 700–900 °C, the widths of the terraces become larger
and the terrace density is decreased with increasing TS. At TS= 900
°C, the width of the largest terrace is ~2000 nm. Fig. 32 shows the
growth rate as a function of reciprocal substrate temperature 1000/
TS. It can be easily found that the substrate temperature dependence
of the growth rate can be divided into three regions with the dif­
ferent activation energies. In the 1000/TS range from 1.04 to 1.22, the
growth rate increases with decreasing 1000/TS (region III). In the
1000/TS range from 0.88 to 1.04, the growth rate is weakly depen­
dent on 1000/TS (region II). Further decrease in 1000/TS results in
the reduction of the growth rate (region I). The regions I, II and III are
identified as a re-evaporation region, a mass transport controlled
region, and a surface controlled region, respectively. The tempera­
ture range of the mass transport controlled region for the ZnO films
grown on the GZO buffer layers is from ~700 to ~875 °C, which is
higher and wider than that for the ZnO films grown on the r-plane
sapphire substrates. Usually the CVD growth of the semiconducting
materials is carried out in the mass transport region because high
B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 31. (a) XRD patterns of the GZO buffer layer and the ZnO films grown on the GZO.
buffer layers at the different substrate temperatures.
accuracy temperature control is not required in this region. There­
fore, the wide range of mass transport controlled region observed for
the ZnO films grown on the GZO buffer layer is convenient for
controlling the composition in the film.The substrate temperature
dependence of growth rate was divided into three regions with
different activation energies, i.e., re-evaporation, mass-transport
controlled, and surface-controlled regions. Scanning-electron-mi­
croscope observations revealed that the films grown at the substrate
temperature in the mass-transport-controlled region exhibited a
terrace-like surface morphology with sharp rock-like structures. J.
Tatebayashi et al. [164] report the formation and optical properties
of Tm, Yb-codoped ZnO nanowires (NWs) grown by sputtering-as­
sisted metalorganic chemical vapour deposition. The ZnO: Tm, Yb/
ZnO core-shell NWs are formed by growing ZnO: Tm, Yb shells on
optimised ZnO core NWs.
Temperature-dependent Hall effect measurements were per­
formed for the undoped CdO films with carrier concentrations (n)
ranging from 2.4 × 1019 to 2.0 × 1020 cm−3 grown on c-and r-plane
sapphire substrates by atmospheric-pressure chemical vapour de­
position using Cd powder and H2O as source materials [165]. Cad­
mium oxide (CdO) with a rock salt structure has a wide direct band
gap of 2.6 eV and a narrow indirect band gap of 2.1 eV and exhibits
n-type conduction. [166] investigated the properties of CdO films
formed by low-pressure chemical vapour deposition as a function of
deposition temperatures ranging from 150° to 450°C.A novel charge-
transport method was used to determine the density-of-states ef­
fective mass of electrons. This mass increased from 0.14 to 0.18 m
25
Journal of Alloys and Compounds 925 (2022) 166511
with carrier concentration. Using this range of values and the re­
duced effective mass, we calculated that the approximate value of
the density-of-states valence-band effective mass is 0.28–0.51 me.
Adelaida Huerta-Barbera et al. [167] have analysed the growth,
morphological and structural characterization of Cd1−xZnxO thin
films grown on rsapphire substrates by atmospheric pressure metal
organic chemical vapour deposition, mainly focusing on the Cd-rich
rock-salt phase for its promising optical and technological applica­
tions. HRTEM images also helped to confirm the presence of the
wurtzite phase in high Zn content samples. The Inverse Fast Fourier
Transform (IFFT) after a filter process on an HRTEM micrograph was
performed on a selected region of the 24.1% Zn content sample, as
shown in Fig. 33. The IFFT image clearly shows the crystalline nature
(single crystal) with an interplanar spacing of about 2.49 Å. Ac­
cording to ZnO pure powder data, the interplanar spacing deduced
from the line profile of the IFFT along the yellow arrow on this region
is very close to the spacing of (1011) planes in the wurtzite structure
of ZnO. The HRTEM analysis on the samples confirms a coexistence
of wurtzite and cubic phases in films grown with Zn contents
≥ 24.1%, as suggested by HRXRD measurements. The fact that the
Zn1−xCdxO bandgap can be potentially tuned in the visible spectrum
by changing the x content provides a path to enhance solar light
absorption in photovoltaics, as well as for other photooptical appli­
cations. Some reports can be found analysing the Zn1−xCdxO alloy
using different techniques, but few of them are focused on the Cd-
rich region, despite the promising applications of this rock-salt
compound as transparent conductive oxide and as a constituent
element in some optical devices [167].
3.7. Atomic layer deposition method
The ALD reactor would produce saturated substrate surface and
growth of ZnO layer by layer [168].
Zn (C2 H5)2 + H2 O ZnO + 2C2 H6
Kazmierczak-Balata et al.,[168] have presented the study of the
morphology and thermal properties of thin ZnO films fabricated by
an atomic layer deposited on n-Si (100) wafers at 200 oC. From
Fig. 34, AFM surface topography and XRD patterns for ZnO poly­
crystalline thin films of thicknesses 118 nm, 110 nm, 38 nm and
15 nm. The main diffraction maxima at angles 32°, 34° and 36°
correspond to the (100), (002) and (101) planes are depicted in the
following graphs for the ZnO sample. The sharp peak located at 33°
corresponds to the Si substrate. The evolution of the (100) peak as
the layer thickness increases is clearly seen in XRD patterns. The
polycrystalline layers exhibit a wurtzite structure with one dom­
inating crystallographic direction [100]. The influence of layer
thickness on surface morphology is clearly seen in the topography
images. Thinner layers are composed of small, spherical grains
evenly distributed within the layer and preferential growth along
the [002] direction. Thicker layers are composed of larger elongated
grains showing a tendency to grow along the [100] direction. The
surface roughness was described by the root mean square coefficient
(RMS). The RMS increased from 1.1 nm to 2.4 nm as the layer
thickness increased from 15 nm to 118 nm, respectively. Surface to­
pography images also indicate grain differences when comparing
pristine and Al doped thin films. The mean surface roughness de­
pended on the number of deposition cycles and varied from 1.1 to
2.6 nm. Thermal conductivity varied from 0.28 to 4.29 Wm−1K−1 and
increased with an increase in average crystallite size. ZnO is applied
as a transparent conductive oxide (TCO), a channel layer in thin film
transistors (TFTs), and a sensitive element in gas and vapour sensors
[169–177]. A ZnO thin film with high coverage and the sharp inter­
face was grown on confined Poly (methyl methacrylate) (PMMA)
templates by atomic layer deposition (ALD) at near room tempera­
ture (35 °C) and investigated by A. Singh et al. [178]. Zinc oxide
B. Amudhavalli, R. Mariappan and M. Prasath Journal of Alloys and Compounds 925 (2022) 166511

Fig. 32. Top (left hand side) and bird’s view (right hand side) SEM images of the ZnO films grown on the GZO films at the different substrate temperatures.

Fig. 33. Filtered-IFFT (right) from a HRTEM micrograph (left) for 24.1% Zn content sample.

26
B. Amudhavalli, R. Mariappan and M. Prasath Journal of Alloys and Compounds 925 (2022) 166511

Fig. 34. AFM surface topography and XRD patterns for ZnO polycrystalline thin films of thicknesses 118 nm, 110 nm, 38 nm and 15 nm.

27
B. Amudhavalli, R. Mariappan and M. Prasath
(ZnO), a type II-VI compound semiconductor with a large direct
bandgap (3.37 eV) and high exciton binding energy (60 meV) at room
temperature, has a wide range of technological applications, in­
cluding semiconductor lasers, light emitting devices, optoelectronic
and photonic devices [179–187].
The thin film transistors (TFTs) with a dual-layer channel struc­
ture combing ZnO thin layer grown at 200 °C and ZnO film grown at
120 °C were fabricated by H. Li et al. [188]. The enhanced perfor­
mance obtained from the dual-layer channel TFTs is due to their
ability to maintain high mobility and suppress the increase in the
off-current at the same time. Owing to oxygen vacancies, the as-
prepared ZnO normally shows n-type semiconducting character­
istics. This has restricted the preparation of high-quality p-type ZnO
and the application of ZnO optoelectronic devices, as reported by Y.
Wang et al. [189]. The temperature range for the self-limited growth
of crystalline ZnO thin films by ALD using diethylzinc and H2O2 was
found to be in the range of 80–150 °C. Commonly used TCOs are
based on SnO2, ZnO, and In2O3. For carrier density values of 1020
cm−3, the upper limits of mobility resulting from intrinsic scattering
are found to be 130 and 55 cm2/Vs for In2O3 and ZnO-based thin film
TCOs, respectively [190–194]. The quantum yield of ALD-ZnO is
shown to be 18-times lower and the luminescence lifetime of the
UV-peak is 14-times shorter compared to bulk-ZnO [195]. Enhancing
photocurrent in solar cells that are limited by sub-optimal electrical
transport in the near infrared region of the electromagnetic spec­
trum can improve energy harvesting efficiency.With ZnO NWs as an
electron transport layer, it can act as a gain medium, amplifying the
field under optical pumping, which enables a lower contact re­
sistance in devices like solar cells by accompanying improvements in
fill factor and open circuit voltage (VOC) [196].
J.R. Bakke et al. [197] have demonstrated the growth of CdxZn1−xO
by atomic layer deposition at 150 °C using diethylzinc (DEZn), di­
methylcadmium (DMCd), and water as the precursors. Both CdO and
CdxZn1−xO are of interest for use in TCOs in the blended CdO (ZnO)/
SnOx system because of their low resistivity, high mobility, and high
transparency. The crystal structure is that of rock salt cubic as op­
posed to the zincblende cubic which is observed for the sulphide
analogue CdxZn1−xO. Further, alloys of CdxZn1−xO ranging from pure
CdO (x = 1) to pure ZnO (x = 0) are demonstrated with bandgaps
varying from 2.3 eV to 3.3 eV.
3.8. Pulsed vapor deposition method
V. Kumar et al. successfully prepared Eu3+ doped ZnO thin films
at different partial pressures of oxygen. Because of the 4–4 f transi­
tion of Eu3 + ions and the excellent properties of ZnO as a host, Eu3+
doped ZnO presents a great opportunity to achieve intense red
emission [198]. H.-S. Koo et al. [199] investigated the structural and
electrical properties of ZnO: Al0.01Sb0.02 thin films grown on the c-
plane sapphire via pulsed laser deposition at 500 °C under different
oxygen partial pressures (0.13–66.66 Pa). Pulsed laser deposition
(PLD) is a very effective method for high-quality thin film fabrication
and provides many advantages, such as the formation of thin films
having the same composition as the target and low contamination.
A. Smaali et al. [200] introduced vanadium as a dopant for trans­
parent and conductive ZnO thin films using multicomponent oxides
of ZnO-V2O5. The XRD patterns show a shift of the (002) peak po­
sition toward lower angles with the increase of V doping implying
the insertion of V toms into the wurtzite lattice. Consequently, the c-
axis lattice parameter calculated from the (002) diffraction angles
rises gradually from 5.164 Å on the undoped film to 5.239 Å on the
4.1 at% doped film is shown in Fig. 35. As can be seen from the SEM
images of the ZnO and VZO films, presented in Fig. 36, the surface
morphology is significantly affected by the amount of vanadium
incorporated in the ZnO films. According to Fig. 36, the top view of
the ZnO surface morphology shows grains with pyramidal-like
28
Journal of Alloys and Compounds 925 (2022) 166511
Fig. 35. XRD patterns of the VZO films. Positions of the diffraction peaks according to
the reference powder diffraction pattern of ZnO (JCPDS 36–1451) are shown at the
bottom.
smooth crests shape forming irregular nanoporous honeycomb-like
surface morphology. By doping vanadium amounts up to 1.6 at%, the
surface morphology becomes more compacted and smoother and
the grain size decreases, a trend that continues up to V contents of
3.2 at%. The lateral grain sizes, derived from the SEM micrographs
are larger compared to the grain sizes calculated from the XRD peak
width which is due to the fact that the latter are measured per­
pendicular to the film surface. O-polar and Zn-polar ZnO films were
grown on c-sapphire by pulsed laser deposition. Positron annihila­
tion spectroscopy studies reveal that the VZn-related defects in the
ZnO films with different polarities are different in structure and their
thermal evolution is different [201]. A.S. Kuzmina et al. present the
results of the study of the composition, structure, and morphology of
ZnO-Co3O4 ceramic targets before and after laser ablation by the KrF
excimer laser. An X-ray diffraction analysis revealed that the com­
position of the targets changes due to the thermal effects of laser
radiation: a new phase of CoO of the cubic structure (a = 4.25) is
formed [202].
For ZnO and indium tin oxide (ITO), O2 are normally used in the
deposition of thin films to achieve lower resistivity and higher
transmittance [203]. In order to obtain higher and stable electrical
conductivity for ZnO without degrading its optical transmission, it is
necessary to introduce an appropriate amount of dopant into it in an
adequate manner [204–213]. However for advanced applications (eg.
flexible optoelectronics, sensors ZnO:Eu thin films deposited at room
or low temperature and exhibiting strong Eu3+ emission at room
temperature is demanding [214,215]. The performance of the het­
erojunction with and without Al-doped ZnO (AZO) layer was more
improved by post-annealing at 200 °C, so that the heterojunction
with and without AZO layer showed power conversion efficiency
(PCE) of 0.61% and 1.5%, respectively. By measurement of external
quantum efficiency (EQE), it was found that the improved PCE of the
heterojunction with AZO layer was attributed to the overall en­
hanced EQE values from ultraviolet to near infrared.
A.M. Mostafa et al. [216] have fabricated the metal oxide thin film
of the CdO structure and mixed it with the ZnO structure. They were
successfully prepared using the second harmonic generation of the
Nd: YAG laser in the evacuated chamber at 450 °C. The FT-IR
B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 36. SEM images of the surface morphology of ZnO (a); and VZO doped 0.9 (b); 1.6(c); 3.2 (d); and 4 (e) at%.
technique showed the presence of the characteristic peaks of the
metal oxides (CdO and Zn) with a slightly shifted characteristic peak
position of the individual peaks of the CdO structure. A.A. Menazea
et al. [217] have enhanced the performance of CdO thin film by
doping it with CuO via a novel way based on making switching of the
metal target between Cd and Cu, which is used to make a deposition
by the Nd: YAG pulsed laser deposition technique. The highest
conductivity achieved for pure CdO thin film is 3500 S/cm (16000 S/
cm for 5% In doped) with a mobility of 200 cm2/Vs. On the other
hand, CdO single crystals have been grown by chemical transport
reaction and vapour phase reaction [218]. From Fig. 37, the SEM
images of these two samples. XRD 2 u scans indicate that the CdO
films on both MgO (100) substrate and the glass substrate have a
(100) orientation. Well-aligned quadrangle grains can be observed in
Fig. 37a, which indicate the epitaxial growth of CdO (100) on MgO
29
Journal of Alloys and Compounds 925 (2022) 166511
(100). At the same time, the quadrangle grains of CdO on glass are
randomly arranged [219]. To the best of our knowledge, no detailed
study of the temperature dependence of the structural and optoe­
lectrical properties of tin-doped CdO using PLD has been conducted
[220 & 221].
Group II-VI metal oxide thin films of cadmium zinc oxide
(CdxZn1-xO) have been deposited using a pulsed laser deposition
(PLD) growth technique in an oxygen-deficient environment as
employed by S. Sharma et al. [222]. The 2D AFM images were taken
over a 5 × 5 µm2 scanning area of the film surface, and root mean
square (RMS) roughness for each sample was recorded as given in
Fig. 38 (a)-(f). It was found that grains pertaining to various scales
were distributed evenly within micro ranges. In Fig. 38 (a), a porous
network of nucleation centers caused by a decrease in the nucleation
energy barrier results in a crater-like surface for sample CZO-1,
B. Amudhavalli, R. Mariappan and M. Prasath
Fig. 37. SEM images of 2.5% Sn doped CdO film on a) MgO (100) and (b) glass.
which extends throughout the film. The peaks in between voids in
the AFM images account for the high concentration of nucleation
centers. However, a 50 °C increase in substrate temperature is ob­
served to promote the formation of spherical grains and smoothen
film surface as RMS roughness reduces from 12.71 nm to 8.34 nm, as
seen in Fig. 38 (d). The morphology of film deteriorates with further
increase in Cd concentration, according to Fig. 38 (e). As the high
speed energetic particles of the laser plume arrive at the surface of
the glass substrate, The effect of cadmium content on the structural,
optical, and electrical properties of the prepared CdxZn1-xO film
samples has been delineated by way of varying CdO composition in
ceramic target samples. The optical band gap is estimated at 3.26,
3.16, and 3.12 eV, respectively, for increasing atomic cadmium con­
centrations in CdxZn1-xO film samples deposited at 250 °C. Im­
portantly, low resistivity films with resistivities in the order of
10 × 10−2 cm were obtained, while electron mobility showed an in­
creasing trend with respect to the presence of cadmium content in
films. This study brings to focus growth aspects of the CdxZn1-xO
material system required for the development of thin film
Fig. 38. 2D AFM images (size 5 µm x 5 µm) of CdxZn1-xO film samples with varying Cdcontent deposited at 250 °C and 300 °C. RMS roughness (SR) values of (a) 12.71, (b) 14.54, (c)
14.82, (d) 8.34, (e) 11.56, and (f) 11.74 nm have been recorded.
30
Journal of Alloys and Compounds 925 (2022) 166511
heterostructures for optoelectronic applications. Preparation condi­
tions of thin films using various deposition methods are listed in
Table 2.
4. Future opportunities for complex oxides
Complex oxides are a branch of metal oxides that have shown
some of the most promising properties across all metal oxides.
Whilst each structure is different, there are always certain properties
that are exhibited by a complex oxide, but they do vary from ma­
terial to material.
Many will be familiar with metal oxides, but within this general
class is a specific category known as complex oxides. Metal oxides, as
a general class, are inorganic materials that contain both oxygen and
metal ions which are often crystalline in nature and possess solid-
state lattices. There are two instances where metal oxides can be
classed as a complex oxide. The first is where the material contains
oxygen and at least two different metallic elements, and the second
 Table 2
Preparation condition of pure and doped ZnO, CdO and CdZnO thin films using various deposition methods.

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

1 0.1 M Zn(NO3)2 320 2h 673 4h 12 – Glass Polycrystalline with a [33]

+ 2NH4OH→Zn(OH2) hexagonal crystal structure
+ 2NH4OH→ (NH4)ZnO2
+H2O+H+→ZnO+NH4OH
2 1.5 mmol 363 6h 773 30 min 3 3.4 µm FTO EB dye dissolved in water [34]
Zn(CH3OO)2.2 H2O did not show a reversible
+ 10 ml ethanol + 0.167 colour change
EB from
B. Amudhavalli, R. Mariappan and M. Prasath

C20H6I4Na2O5·H2O
3 0.1 M 363 50 min – – 11.4 – glass Eg= 3.3 and 3.2 eV. This may [35]
Zn(CH3OO)2.2 H2O be interpreted by the
+ 0.1 M Cd decrease of the film
(CH3OO)2.2 H2O thickness
4 0.1 M 358 2h 673 3h – 120 nm glass Wide Eg nature of ZnO and [36]
Zn(CH3OO)2.2 H2O presence of atomic level
+ (CH2)6N4 defects in the crystal
structure
5 0.1 M Zn(CH3OO)2.2 H2O 400 10 min – – 7 225–1138 glass Grain boundary resistance [37]
nm decreases with the
increasing ammonia
concentration up to
500 ppm and the maximum
sensitivity is found to be 1.7

31
6 Zn(NO3)2.6 H2O+HMTA
7 [Zn(NH3)4]2++H2O→Zn2+
+NH4++OH-→Zn(OH)2→
ZnO+H2O
8 0.02 M ZnSO4 + 1.5 M
NH4NO3 + 0.925 M
KOH→Zn(OH)3-→ZnO
+H2OS
0.02 M ZnSO4 + 1.5 M
NH4NO3 + 0.925 M
KOH→Zn(NH3)42→ZnO
+NH3 +H2O
9 Zn(NO3)2
+C6H12N4→[Zn
(C6H12N4)]2++2OH-→
ZnO+H2O+ C6H12N4
10 0.1 M
Zn(NO3)2.6 H2O+HMTA
(C6H12N4)-→ZnO+H2O
+ C6H12N4
for 500 ppm of ammonia
333–373 2h 773 180 min – 100 nm glass Deposition time of 180 min [38]
can be used as a possible
photoanode for dye-
sensitized solar cells.
393 1h 673–1073 1h 10 500 nm glass Direct band gap at 3.4 eV, a [39]
high bonding energy
(60 mV) and a high thermal
and mechanical stability at
room temperature.
298–318 – – – 11.35–12.30 40–72.5 glass Optical band gap ranged [40]
nm from 3.31 eV for Zn(OH)2 to
3.41 eV for ZnO. It is
confirmed that the ZnO
compound exhibited the
highest crystallinity
385 15–60 min 400 1h – 100 nm ITO The average grain size and [41]
roughness of ZnO layers
obtained 30–42 nm and
4.786 nm.
333 2h – – – 100 nm Silicon The n-ZnO/p-CuO [42]
heterojunctions is attributed
to the combination of both
narrow and wide bandgap
semiconductor in such
structures which also leads
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

to the increased efficiency of

the devices.
11 25 mM 363 2h > 673 1h – 400 and Si Wafer The results indicated that [43]
Zn(NO3)2.6 H2O+ 25 mM 800 nm the annealing process
HMTA significantly modified the
(C6H12N4)-→ZnO+H2O crystalline structure, both at
+ C6H12N4 the bulk and at the surface.
12 0.5 M Cd 363 4h 500 1h – – glass Band gap of the CdO was [44]
B. Amudhavalli, R. Mariappan and M. Prasath

(CH3COO)2.2 H2O found to decrease with

+ (H2NCH2CH2OH) increase in molar
+ 10 ml 2- concentration
methoxyethanol
II. Preparation of pure and doped ZnO, CdO and CdZnO thin films using spray pyrolysis method
Sr.No. Bath composition Deposition Deposition Pressure/ Nozzle pH Film Substrates Remarks Ref.
temperature time Flow rate distance thickness used
(oC) (cm)
13 Zn(CH3COO)2.2 H2O→Zn 250,350 5 3 ml/min 8 – 25 nm glass The TFTs show excellent [45]
(OH)2 and 400 stability with a low
+ 2CH3COOH→ZnO+H2O threshold voltage shift of
+CH4 +CO2 0.1 V under gate bias stress.
14 0.1 M 250,300,350,­ – 10 ml 5 – 300–465 glass ZnO films prepared which [46]
ZnC4H6O4.2 H2O+CH3OH 400,450, 500 nm have a c-axis position is
perpendicular to substrate
surface are applicable in

32
solar cells, optical windows
and gas sensors.
15 The mixture of 8.8 g of 200, 275,400 30, 60, 120, 6 ml 15 – 2.0 ± 0.­ glass ZnO films deposited by [47]
zinc acetate dihydrate, 180 min 4 µm. spraying of nanoinks
40 ml of ethylene glycol, containing synthesized
1.76 g of nanocrystals by polyol
polyvinylpyrrolidone method possess
fundamental properties
suitable for application in
the flexible solar cells and
thermoelectric generators.
16 4Zn(CH3COO)2 425 2 min 5 ml – – 300 nm glass ZnO films were synthesized [48]
+ 2 H2O→Zn4O via chemical spray
(CH3COO)6 technique and irradiated by
+ 2CH3COOH→4ZnO electron beam at dosages of
+ 3CH3COCH3 + 3CO2 5 kGy, 10 kGy and 15 kGy
17 0.1 M zinc 460 5 min 4 ml/min 27 4.7 – ITO glass The ZnO:2%Ag used in PEC [49]
acetate+ 2-Propanol has shown an enhanced
+ acetic acid photoelectrochemical
performance of magnitude
Voc = 0.38 V, FF = 0.27, and
η% = 0.45%.
18 0.2 M 450 – Pressure:1.5 kg/ 30 mm – 360–448 glass The sensor response is [50]
[Zn(CH3COO)2⋅2 H2O] cm2 nm remarkably high (97.07%) for
+ 10 ml (CH3OH) + 0%, 3% Er-doped ZnO film and is
1%, 3% and 5% [Er(NO3) three times higher than that
3⋅5 H2O] of the undoped ZnO film.
19 100% dissolved Zn 350 ± 10 25 min Pressure:6×104 30 – 291, glass The increasing of the Sn [51]
(NO3)2 Pa 220,240, amount at fixed Al
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

99% dissolved Zn(NO3)2 Flow 306,303, concentration showed a

+ 1% dissolved Al(NO3)3 rate:2 ml/min 300 nm slight loss of crystallinity of
98.75% dissolved Zn the ZnO films.
(NO3)2 + 1% dissolved Al
(NO3)3 + 0.25% dissolved
SnCl2
98,5% dissolved Zn
(NO3)2 + 1% dissolved Al
B. Amudhavalli, R. Mariappan and M. Prasath

(NO3)3 + 0.5% dissolved

SnCl2
98.25% dissolved Zn
(NO3)2 + 1% dissolved Al
(NO3)3 + 0.75% dissolved
SnCl2
98% dissolved Zn(NO3)2
+ 1% dissolved Al(NO3)3
+ 1% dissolved SnCl2
20 0.1 M ZnCl2 + H2O → 500 – – 30 – 370 nm Soda lime The optical band gap of ZnO [52]
ZnO↓ + 2HCl↑ thin films is decreased,
while the Seebeck
coefficient is increased
significantly with an
increased concentration of
Al-dopant in ZnO thin films.

33
21 0.2 M ZnCl2 + 0.2 M 450 10 min – – – 150 nm Silica both lattice parameters and [53]
NH4VO3 +H2O → ZnO:V↓ crystallite size decrease
+ 2HCl↑+NH3 with increase V doping
percentage indicating the
substitution of vanadium
V4+ and/or V5+ ions to Zn2+
ions in the ZnO host lattice
22 0.1 M Zn(CH3CO)2.2 H2O 400 – Pressure:15 Psi 15 – 20 nm glass Electrical stabilities can be [54]
+ Methanol considered a significant step
to address
commercialization of the
MOS FETs based on the
spray pyrolysis process.
23 Zn(NO3)2 + methanol 90 0.65 g/min Pressure:1 bar 15 – 5–10 µm Stainless high potential to increase [55]
steel the membrane performance
by further optimizing the
reaction parameters.
24 20 ml C10H14O4Zn·H2O 400 25 ml/ Flow rate:15 min – – 100, 230, Soda lime The photocatalytic [56]
15 min 305, glass efficiency is shown to
720 nm decrease with increasing
deposition time, which is
explained by the increase in
the 24structural and surface
defects with the deposited
ZnO thin film thickness
25 0.05 M ZnCl2 +NH4OH 400–500 – 2.4 ml/min – 10 – glass The formation of ZnO [57]
occurred upon the thermal
decomposition of both
precursors in a liquid form
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

which is favourable for

growth of high purity ZnO
structures
26 0.05 M ZnCl2 + 2,5,7% 450 6 min 2 ml/min 40 – – glass All sprayed films are [58]
(CH3CO2)3Y.xH2O polycrystalline with a
hexagonal wurtzite
structure and strongly
oriented towards the [002]
B. Amudhavalli, R. Mariappan and M. Prasath

direction
27 0.5 M 300 15/15 s, 30/ – – – – glass N-doping by using N2 gas [59]
(Zn(CH3COO)2.2 H2O) 30 s, and source was found effectively
+ 0.5 M 60/60 s contributing towards the
(NH4(CH3COO).2 H2O) achievement of p-type
conductivity without the
contribution of oxygen
vacancy defects as well as
defect complexes
28 Zn(CH3COO)2.2 H2O and 450 30 min 2 ml/min 28 – 500–600 Glass At and below room [60]
0–10%Co nm temperature, all deposits
(CH3COO)2.4 H2O showed paramagnetic
nature.
29 0.4 M (Zn 400 10 2 ml/min 15 – – p-type The Er-doping process in the [61]
(O2CCH3)2.2 H2O Si (100) ZnO NC films will be useful
+ acetic acid (CH3COOH) for developing the strategy

34
and methanol (CH3OH) and obtaining ZnO:Er NC
in the volume films with the tailored
proportion parameters.
10:10:80 + 1,2,3,5% of
((CH3CO2)3Er xH2O
30 Zn(NO3)2 + H2O→ Zn2+ + 400 – 45 slpm 10 – 10 µm stainless ZnO coatings had good [62]
2NO3- + H2O steel response and recovery when
exposed to UV light.
31 0.2 M solution of zinc 375, 400, 450 6 – – – 117,139,1­ Soda lime Results confirm the [63]
acetylacetonate 69, glass potential application of
dissolved in a mixture of 220,236,­ ultrasonically ZnO thin films
acetic acid, water, and 254 nm for photocatalytic
methanol applications
(100:100:800 vol
proportions
32 (Zn (CH3OO)2.2 H2O) 350 5–6 2 ml/min 20 – 200 µm Glass X-ray diffraction analysis, [64]
+ 1,2,3,4,5% the preferred (002) oriented
(SrCl2.6 H2O). hexagonal phase of ZnO was
confirmed for all samples
studied
33 10.97 g Zinc acetate and 400,450,500 5s Pressure:5 Psi 30 – 82–138 ± Soda lime The average size of the [65]
ethanol 7 nm glass crystallite in the samples
range from 22.88 nm to
36.52 nm; meanwhile the
average particle size varied
from 50 to 230 nm
34 0.1 M zinc nitrate 400 5 1 ml/mn 25 – 750,1150­ Glass Undoped ZnO shows [66]
+ 1,2,3% aluminium ,1100, maximum sensitivity at
chloride 1200 400 °C for higher
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

concentration of CO2
whereas aluminium doped
samples show maximum
sensitivity either at 350 °C
or below for all CO2
concentrations
35 Zn 450 – Pressure:0.5 bar 25 – – glass Spray pyrolysis, can be used [67]
(COOCH3).2 H2O)+H2O as a suitable material for
B. Amudhavalli, R. Mariappan and M. Prasath

+ 1,5,10% FeCl3 optoelectronic applications

36 0.05 M 400 2.5 2 ml/min 15 – – glass Al doping in ZnO results in [68]
(Zn(CH3OOH)22 H2O) nanostructure ZnO films
+ 0–5% (Al(NO3)3.9 H2O) with high surface density
and better electrical
conductivity, which can be
useful in many applications,
e.g. photocatalytics,
transparent
conductive films.
37 Cadmium acetate [Cd 250 ± 5 30 2 kg/cm2 25 – – Soda lime low resistive and high [69]
(CH3(COO)2)] + dopant glass mobility of 1.5% Al doped
(0.5–1.5 wt%) aluminum CdO film exhibited
nitrate nonahydrate [Al pronounced sensitivity,
(NO3)3⋅9 H2O] 32.12%, is due to its higher
specific surface area and as

35
well as existence of more
defective sites.
38 0.09 M CdCl2 + [0.01 M 350 ± 5 – 1.5 kg/cm2 30 mm – 620, 570, glass The optical band gap was [70]
ZnCl2 + 0, 0.5, 1.0, 1.5 wt 540, found to be increased by
% Tb(NO3)3⋅5 H2O)] 530 nm increased Tb concentration.
39 0.3 M cadmium acetate 400 Annealed:1­ Flow rate: 25 – 0.6, glass The phase confirmation and [71]
+ [ water + methanol h 3 ml/min 1.3, 2 µm detail structural parameters
mixed ratio 2:3] were investigated using XRD
analysis. Spherical
nanoparticles like
morphology having size
7–8 nm of CdO film was
observed
40 0.1 M Cd(CH3COO)2 400 3 min 3 ml/min 22 – 0.68 µm glass The stability of the CdO thin [72]
+ 3 H2O → CdO + CH4 film electrode was tested by
+ 4 H2 + 3CO2 continuous charge-
discharge cycle up to 1500
cycles, signifying the
potential of as fabricated
CdO film electrode for
energy storage application.
41 0.1 M Cd(NO3)2.4 H2O 400 3 min 2.5 ml/ min 25 – 1000 nm glass CdO structure with the [73]
+dopant 1,2,3 molar (200) preferential
ratio of Pb(NO3)2 orientation and the cubic
structure with planes of
(111), (200), (220), (311) and
(222) independent of Pb
dopant
42 200–300 20 min (14.7 ×104 Nm−2) 1 – 548 nm glass [74]
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

0.2 M [Cd X-ray diffraction study

(CH3(COO)2)]·2 H2O showed that all these thin
+ 2 at% SnCl2.2 H2O films were polycrystalline
with major reflection along
(1 1 1) plane and the
crystallite size had
increased at elevated
annealing temperatures
B. Amudhavalli, R. Mariappan and M. Prasath

42 Cd(CH3COO)2.2 H2O 300 2 min 5 ml/min and 105 21 – 150 nm glass yttrium (Y) is an effective [75]
+ H2O → CdO + CH4 N/m2 dopant element for CdO to
+ 3CO2 introduce advance opto-
Y(CH3COO)2.4 H2O+ Cd electronic devices
(CH3COO)2.2 H2O+ H2O
→Y: CdO + CH4 + 3CO2
44 0.05 M Cd 300 ± 5 – 45 kg/cm2 30 – 300 ± 10 glass Co- doped CdO thin films [76]
(CH3COO)2.2 H2O nm indicates that the prepared
+ dopant (0.25, 0.50, films are the potential
0.75 and 1.0 wt%) of candidates for the gas
CoCl2.6 H2O sensing and the
optoelectronic applications
45 0.666 g of cadmium 300 – 45 kg/cm2 30 – 350 glass Ru doped CdO films as [77]
acetate dehydrate compared to CdO film
+ ruthenium (III) promises the potentiality of
chloride trihydrate (0.1. sprayed Ru doped CdO thin

36
0.125, 0.150, 0.175, films as the TCO layer in
0.2 wt%) opto-electronic and solar
cell devices.
45 0.1 M cadmium acetate 300 ± 5 – 45 kg/cm2 30 – 400 glass XRD study shows cubic [78]
+ doping 0%, 1%, 3% and structure of grown films.
5% of praseodymium Band gap values are in range
(III) chloride of 2.42–2.20 eV.
hexahydrate
(PrCl3.6 H2O)
47 [Cd (CH3COO)2.2 H2O] 350 – – 30 – 600, 720, glass The Al/Eu-nCdO/p-Si/Al [79]
+ dopant (0, 1, 3 and 740 and heterojunction diode can be
5 wt%) EuCl3,6 H2O 690 nm used for the photo sensor
for 0%, 1%, and other optoelectronic
3% and 5% applications
Eu: CdO
thin films
48 0.2 M cadmium acetate 200 – 14.7 × 104 Nm−2 1 – 540–575 glass The maximum conductivity [80]
dehydrate+ dopant 0, 2, nm was observed at the 6 at% of
4, 6 and 8 at% doping which is less than
Ammonium that of CdO:F films reported
fluoride (NH4F) in earlier studies.
49 0.05Mcadmium acetate 250 – 2 kg/cm2 35 – – p-Si and The fabricated n-CdO/p- [81]
+ (0.1, 0.2, and 0.3 mM) glass silicon diode structure
of stannic chloride showed improved
(SnCl4) photoresponse due to the
inclusion of Sn
50 0.2 M cadmium acetate 200 – − 10.8, 12.7, 14.7, 1 cm – 360, 473, glass CdO thin films were [82]
+ 1:3 ratio of isopropyl 16.7 and 540, 500, polycrystalline in nature
18.6 × 104 N m−2) 481 nm along with cubic structure
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

alcohol and de-ionized

water
51 0.05 M [Cd(CH3COO)2] 400 – 2 kg/cm2 25 – 726/0d glass CdZnO thin film coated from [83]
+ 0.05 M [Zn(CH3COO)2] ay, 734/ 3 days aged solution
1 day, exhibited better structural,
711/2 day, morphological, optical and
698/ electrical properties, which
3 day, make them suitable for
B. Amudhavalli, R. Mariappan and M. Prasath

706 optoelectronic applications.

/4 day
52 cadmium acetate 375 5 min 12 × 104 Nm−2 30 – 460, 443, glass XRD studies revealed that [84]
(0.05 M) + (0, 2, 4, 6 and 439, 427, film crystallinity improves
8 wt% Zn) 446 nm with annealing temperature.
All the films exhibited cubic
crystal structure with a (111)
preferential orientation
53 cadmium chloride 400 2 ml/min 2 bar 30 – 600 nm glass Low cost materials and ease [85]
+ Zinc diacetate of production of CdxZn1−xO
dihydrate thin films makes it a
potential candidate for
ethanol sensors.
III. Preparation of pure and doped ZnO, CdO and CdZnO thin films using sol-gel spin and dip coating method
Sr.No. Bath composition pH/ Molarity Spinning Spinning Preheat Preheat (P) Film Substrates Remarks Ref.
speed time (sec) (P) /Annealing thickness used

37
(rpm) /Anneali­ (A) time
ng (A)
tempera­
ture (oC)
54 Zn(CH3COO)2.2 H2O + monoethanolamine (MEA) –
+ ethanol
4000 30 P: 300 P:10 min, – Si, Glass The FESEM [86]
A:400,500,6­ A:1 h micrographs
00 clearly manifest
that nitrogen
and gallium co-
doping
significally
modifies the
film
morphology,
the wrinkle
network of
undoped ZnO
films is
surprised and
closed packed
grained
structures are
observed
55 [Zn(CH3COO)2.2 H2O] + monoethanolamine (MEA) 0.2,0.3,0­
+ isopropanol 4,0.5,0.6
M
2000 30 P:200, A:450 – Glass [87]
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

P:10 min, The

A:1 h concentration
of the sol can
have a
considerable
effect on the
efficiency of the
solar cells
B. Amudhavalli, R. Mariappan and M. Prasath

where such
studies can be
useful.
55 zinc acetate dihydrate – 3000 30 P:200 P:10 min 2.5 µm Pt/Ti/ The sol-gel technology [88]
+ polyvinyl alcohol A:600,65­ A:45,30,30,50 SiO2/Si made the vanadium doping
+ 2.5% doping vanadium 0,700,750 min more uniform and sufficient,
thus improving the
piezoelectric properties of
the thin film.
57 [Zn(CH3COO)2⋅2 H2O] 0.5 M 3000 30 A:400 A:3 h 320 ± 30 Glass all the films, 1:3 at% Sn-In [89]
+ 2-MOE, C3H8O2 + MEA, nm co-doped ZnO film (1T3IZO)
C2H7NO + For dopants exhibits the optimum
{tin (II) chloride transmittance and lower
dehydrate [SnCl2⋅2 H2O] electrical resistivity.
+ indium (III) nitrate
hydrate [In

38
(NO3)3⋅xH2O]}
(0 at% Sn + 1 at% In),
(1 at% Sn + 1 at% In),
(1 at% Sn + 3 at% In),
(3 at% Sn + 1 at% In), and
(1 at% Sn + 0 at% In).
58 [Zn(CH3COO)2⋅2 H2O] 0.5 M 3000 30 P:200, P:15 min, A:3 h 320 ± 40 Glass The direct energy band-gap [90]
+ (2-MOE, C3H8O2) + + A:400 nm has been found to be least
MEA, C2H7NO + For value (3.20 eV) for the
dopants {tin (II) chloride 1T1GZO film, whereas the
dehydrate [SnCl2⋅2 H2O] refractive index is least
+gallium (III) nitrate (2.12) at the wavelength of
hydrate (Ga 600 nm for the 1T3GZO film
(NO3)3⋅xH2O)}
1 at% Ga-doped, 1 at%
Sn-doped, (1 at% Sn þ
1 at% Ga) co-doped, (1 at
% Sn þ 3 at% Ga) co-
doped and (3 at% Sn þ 1
at% Ga)
59 Zn(CH3COO)2.2 H2O 0.5 M – – P:250, P:10 min, A:1 h 120 nm Glass Film optical band gap has [91]
+ Diethanolamine (DEA) A:600 been affected slightly with
+ 2-methoxyethanol + 0, doping amount from ~
1, 3 (at%) Al(NO3)3.9 H2O 3.33–3.38 eV. Refractive
index tended to decrease
slightly with the increasing
of the Al concentration. the
sol–gel dip coating process
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

displayed valid performance

for semiconductor device.
60 Zinc acetate dihydrate pH:10, 0.5 M 3000 30 P:100, P:10 min, A:1 h – Glass Excluding the effect of film [92]
+ [2- propanol, A:450 material absorbance, the
stabilized with light rapping impact can be
monoethanolamine] structural, due to the
pyramid-like textured
structure, favourable for
B. Amudhavalli, R. Mariappan and M. Prasath

application in solar cells

61 [Zn(CH3COO)2.2 H2O] 0.3 M – – A:400 A:1 h 150 ± 20 Glass undoped and Al doped ZnO [93]
+ dopant Aluminum nm nanocrystalline thin films
chloride hexa-hydrate were prepared on glass
[AlCl3.6 H2O] + ethanol substrate by sol–gel dip
+ Diethanol coating technique. This
amine (DEA) study may open a versatile
route to achieving high
efficiency of photocatalytic
activity of ZnO
62 zinc acetate dihydrate + Monoethanolamine (MEA) 0.5 M
+ isopropanol
4000 40 P:200, A:600 A:1 h 100 nm ITO/ glass The structure of [94]
Si:13–17 µm and Si ZnO thin films
deposited by
the sol-gel

39
technique
showed the
films to have
hexagonal
wurtzite
structure, with
a crystallite size
of 48 nm.
63 Zn(CH3COO)2∙2 H2O 0.5 M 2000 30 P:200, P:10 mn, A:1 h 500–550 Glass Sm- and La-doped ZnO thin [95]
+ LaCl3∙7 H2O + SmCl3 A:500 nm films have shown better
+ monoethanolamine photocatalytic degradation
(MEA) efficiency for methylene
Concentration:0.2, 0.4, blue under solar light
0.6, 0.8, 1,3, 5 wt% irradiation.
64 Zinc acetate dehydrate + monoethanolamine (MEA) 0.5 M
+ 3,5,7 at% cerium
nitrate hexahydrate
+ 1 at% aluminum
nitrate Nonahydrate
+ Isopropanol
3500 30 P:200, A:450 P:5 min, 0.38 µm Glass The effect of [96]
A:30 (Ce, Al) co-
doped ZnO
films on the
structural and
optical
properties has
been studied,
and the
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

electrical
characteristic of
the fabricated
Schottky diode
devices are
investigated
65 Zn(CH3COO)2∙2 H2O + monoethanolamine (MEA)
+Ethanol
B. Amudhavalli, R. Mariappan and M. Prasath

3000 30 P:300, A:800 P:5 min, 30,100, 190 nm Glass The surface of [97]
A:1 h the ZnO layer in
contact with
the ambient
contains active
sites, resulting
in
chemisorption
of ambient
gases such as
oxygen prior to
the deposition
of subsequent
layers
66 ZnC4H6O4.2 H2O 0.3 M 1000 30 A:450 A:3 h 119 nm Glass ZnO nanofilms have [98]
+ C2H6O wurtzite structure

40
67 Zn(CH3COO)2.2 H2O 0.1 M 2200 30 P:300 P:30 min, A:1 h 200 nm Glass Al-Sn codoped ZnO thin [99]
+ 1,2,3,5 at% Al(NO3)3 A:500 films were polycrystalline
+ 5 ml (CH3)2CHOH and exhibited preferential
+ 5 ml growth along c-axis. These
CH3CH2OH+mono- thin films werea mixture of
ethanolamine (MEA) two phases with a
transparency over 80% in
visible range, this sample
may be promising to
fabricate thin films
transistors (TFTs)and
Ultraviolet light emitting
diodes (UV-LEDs).
68 Zm (CH3COO)2.2 H2O+ 2 – – 5 min P:150, P:20 min, A: 2 h 4.8 µm, Glass The Morphology of ZnO thin [100]
(NH2CH2CH2OH)→ A:500 75 µm films are change with
2 H2O annealing temperature and
+CH3CONHCH2CH2OH2 SEM image represented by
+Zn(OH)2→ZnO+H2O different ganglia-like hills.
These properties are useful
in using these dopant films
as gas sensor.
68 Zinc acetate 0.5 M 3000 40 A:320 A:4 h 100 ± 10 Si Wafer A hexagonal wurtzite [101]
dehydrate+ Ethanol+ 2- nm structure with the (002) c-
propanol axis orientation in the film
+ Ethanolamine growth direction was
evident along with a dense
microstructure of
homogeneously distributed
grains.
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

70 Zn(OAc)2•2 H2O+Ga 0.4 M 2000 30 P:100,15­ P:5 min, A:2 h 250 nm glass Well-formed GZO thin films [102]
(NO3)3•xH2O+C2H6O 0,200,250 prepared by sol-gel route
+Diethanolamine (DEA) A:350 can be achieved by an
or 400 assistance of baking process
during coating at certain
temperature that can lower
the operating temperature
of annealing process.
B. Amudhavalli, R. Mariappan and M. Prasath

71 (Zn(CH3COO)2.2 H2O) 3000 20 P:310, P:10 min A:0.5 h 180 nm Soda lime optical properties imply the [103]
+ (C3H8O2) A:500 glass decrease of optical bandgap
+ (HOCH2CH2NH2, MEA with the increase of Nb
+ content
1 at%(AlCl3.6 H2O)
+ 1–4 at% (NbCl5)
72 Zn(CH3COO)2•2 H2O – – 10 mm/min A:400 A:60 min 30–90 nm glass The SEM and AFM data have [104]
+ isopropanol and 500 shown that all films are
+ monoethanolamine nanocrystalline and the
(MEA, HOCH2CH2NH2, postdeposition annealing of
Zn(CH3COO)2•2 H2O the films causes an increase
+ isopropanol of the grain size from 13 to
+diethanolamine (DEA, 20 nm in the films annealed
HN(CH2CH2OH)2, at 400°C to 20–40 nm in the
films annealed at 500°C.
73 (Zn (CH3COO), 2 H2O) 0.4 M – 1.5 cm/min P:200, P:10 min, A:1 h – glass All the films are crystallized [105]

41
+ ethanol A:500 in a ZnO hexagonal wurtzite
+ monoethanolamine structure and are highly c-
(MEA, C2H7NO + gold axis oriented.
(III) chloride hydrate
(AuCl4·H2O)
74 Zinc acetate + ethanol 0.5 M 2000 40 P:200, P:5 min, A:2 h 151 nm ± Glass ZnO thin film sensor shows [106]
+ m-cresol A:400 10 nm fast response and recovery
time of 2 s and 137 s
respectively upon 100 ppm
NO2 exposure with excellent
stability (68%) and
repeatability.
75 [Zn(CH3CO2)2.2 H2O] – – – P:100, P:10 min, 80, 167, Glass and The Auger spectra gave an [107]
+ 2,5,10 wt% Cd A:500 A:120 min 220, silicon idea of the thickness of the
(CH3CO2)2.2 H2O + 30 ml 240 nm films with respect to the
2-Methoxyethanol pickling time, and this
+ 0.6 ml Ethanolamine confirms the RBS result
76 Zn(CH3COO)2.2 H2O 0.5 M 1500 60 s P:120, P:10 min, A:2 h 127,154,1­ Glass XRD analysis revealed a [108]
+ 20 ml 2- A:450 76,192 preferential c-axis growth
Methoxyethanol and with a hexagonal Wurtzite
+ (Mg/Zn) molar ratio of 205 nm structure and an increase in
0,1,5,10,15% Mg grain size with increase in
(NO3)2.6 H2O Mg concentration. Mg
doping on the ZnO thin films
for possible optoelectronics
applications.
77 [Zn + monoethanolamine; MEA 0.7 M
(CH3COO)2.2 H2O]
+ 7,10,12.5 mol% [Mn
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

(CH3COO)2.4 H2O]
+ Isopropanol
2800 30 P:250, A:500 P:10 min, – Glass Grain size and [109]
A:1.5 h surface
roughness were
decreased with
x, leading to the
decrease of the
B. Amudhavalli, R. Mariappan and M. Prasath

average
transmittance
78 cadmium acetate + monoethylamine (0.5 M) –
dehydrate +dpoing (1%,
2.5%, 5% and 10% wt%.)
Erbium nitrate + 0.5 M 2
methoxy ethanol
1500 30 P:120, A:450 P:10, A:2 h – FTO glass Indirect band [110]
gap values are
changing with a
variation of
doping from
2.85 to 2.97 eV.
79 Cadmium acetate 0.1 M, 0.2 M, – – P:150, P:5 min, 85 nm Soda lime The crystallinity of the [111]
dihydrate + methanol 0.3 M, 0.4 M A:450 A:60 min glass structure maintains the
(CH3OH) + mixture and 0.5 M ideal form, while the band

42
(H2O2, NH3 and gap of CdO thin films
H2O, 1:1:5) decreases with increasing
molarity.
80 Cd(CH3COO)2.2 H2O 0.5 M 1500 30 P:120, A:2 h – FTO glass The increased energy gap [112]
+ doping (1%, 2.5%, 5%, A:450 and high values on
7.5%, and 10 wt%) La nonlinear constants make
(NO3)3.6 H2O the fabricated films of
+ 2-Methaoxy ethanol La:CdO/FTO an important
contender for optoelectronic
devices.
81 Cd(CH3COO)2.2 H2O 0.3 M 3000 25 P:200, P:10 min, A:1 h – Soda lime Optical band gap value of [113]
+ [CH3OCH2CH2OH] A:500 glass undoped-CdO continually
+ [NH2CH2CH2OH] declines, but the Urbach
+ doping (2, 4, 6, 8, 10 at energy values increases
%) [(Si(CH3)3)2] with Si-dopinglevels.
82 Cd(COOCH3)2.2 H2O 0.2, 0.5, 0.8 M 3000 30 P:200, P:10 min, A:1 h – Glass The electrical analysis also [114]
+ C3H8O2 +C2H7NO A:450 suggested a good electrical
conductivity for the 0.5 M
CdO thin film.
83 Cadminum acetate Volume ratios 1500 30 P:150, P:10 min, A:1 h 200 nm glass The optical band gaps for [115]
dehydrate + zinc acetate 1:1, 1:3, A:400 CdZnO (3:1), CdZnO (1:1),
dehydrate and 3:1. and CdZnO (1:3) were found
+ 2-methoxyethano to be 2.80 eV, 2.49 eV, and
+ethanolamine 2.52 eV
84 [Cd(COOCH3)2.2 H2O] 0.5 M Dipping – P:275, P:10 min, A:1 h 136–143 glass The optical band gap of the [116]
+ [Zn(COOCH3)2.2 H2O] speed A:450 nm films was tuned from 3.36 to
+ (C3H8O2 + 106 mm/ 2.28 eV by varying x from 0
(C2H7NO, MEA) min to 1.
85 0.5 M 2500 60 P:10 min, A:1 h 200 nm glass [117]
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

[Cd(COOCH3)2.2 H2O] P:240, Highly conducting and low

+ [Zn(COOCH3)2.2 H2O] A:450 optical bandgap thin films
+ (C3H8O2 + may be suitable for
(C2H7NO, MEA) applications in solar cells
and optoelectronic devices.
86 [Cd(COOCH3)2.2 H2O] 0.5 M Dipping – P:275, P:10 min, A:1 h 140 nm Soda lime The carrier concentration [118]
+ [Zn(COOCH3)2.2 H2O] speed A:450 glass and carrier mobility of the
+ (C3H8O2 + 106 mm/ samples were increased
B. Amudhavalli, R. Mariappan and M. Prasath

(C2H7NO, MEA) min with Cd ratio whereas in the

same time, the resistivity of
the films was decreased
87 [Cd(COOCH3)2.2 H2O] 0.2 M/l 3000 1m P:250, P:30 s, A:1 h – glass All the films are exhibited [119]
+ [Zn(COOCH3)2.2 H2O] A:300–8­ the wurtzite crystal
+ (C3H8O2 + 00 structure. The systematic
(C2H7NO, MEA) study of ZnCdO thin films at
various annealing
temperatures exposed that
the crystallinity, grain sizes,
bandgap and
photoluminescence
enhanced with annealing
IV. Preparation of pure and doped ZnO, CdO and CdZnO thin films using electrodeposition method
Sr.No. Bath composition Molarity/pH Potential Time (min) Bath (B) Bath (B) / Film Substrates Remarks Ref.
(V) /Preheat­ Preheated (P) thickness used

43
ed (P) /Annealed
/Anneale­ (A) time
d (A)
tempera­
ture (oC)
88 Zn(NO3)2.6 H2O 0.005 M -0.7, − 1.0, 20 65 – ITO The transformation in [120]
− 1.3, − 1.3 morphology is postulated to
be caused by the attack of
Cl− ions on the surface of
ZnO nanoparticles
89 Zn(CH3OO)2.2 H2O+Ga – 10 10 min P:100, P:10 min, A:1 h – FTO, with DRS spectra illustrate more [121]
(NO3)3·H2O+CH3OH/ A:500 15 Ω/sq absorbance in the range of
MeOH+C2H5OH/EtOH+N sheet 350–750 nm for GZO1
(CH2CH3)3/TeA resistance rather than UZO and the
Concentrations: 0.25, band gap is slightly blue
0.5, 1, and 2 mol% of shifted to 3.28 eV
Ga/Zn+Ga
90 ZnCl2 0.005 M -0.8 10 min B:75, A:60 min 521, 536, FTO, with Application of annealing [122]
+ KCl+ CuSO4.5 H2O A:350 543, 15 Ω/sq treatment results in slightly
+ C3H6O3 552 nm sheet increased photo-electrical
+ NaOH+ dimethyl resistance properties for the
sulfoxide heterojunction solar cells,
dueto the strong interface
properties and the defects in
ZnO lattice which reduce
the recombination at
interface
91 5 mM -1.0 10 min B:75 – – ITO coated Mn doped ZnO thin films of [123]
glass Zn1 −xMnxO (x = 1%, 3%, 5%,
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

Zn(NO3)2.4 H2O + 0.3 M samples 7% and 10%) have been

KCl+ (1–10 wt%) (10–15 Ω/ synthesized by using
MnCl2.2 H2O sqr, 2 cm2 electrodeposition technique
surface area
92 ZnCl2 + 1 M KCl 0.5 mM -1.0 30 min B:80 – – ITO The nanowalls are grown [124]
into the oxygen dislocations
on Zn-terminated ZnO
wafer.
B. Amudhavalli, R. Mariappan and M. Prasath

93 Zn(NO3)2.4 H2O 8 mM -1.4 20 min B:70, A:30 min 55 nm ITO The SEM image obviously [125]
+ 16 mM KCl A:400 displays that the as-
prepared ZnO has flower-
like structure
94 2 Zn(NO3)2 + 2NaOH → 0.025 M, 7 M -0.4 – P:150 P:16 h 1, 4 µm FTO ZnO rod arrays/Cu2O thin [126]
Zn(OH)2 + 2NaNO3 film heterojunction is a
+ 6 H2O →ZnO↓ + H2O promising device on
fabrication of low cost and
high-performance LED with
white electroluminescence.
95 Zn(CH3COO)2 0.25 M -1.0 10–20 min B:70, B:15 min 260 nm ITO glass Nanorods have larger mean [127]
P:100, A:20 min diameter of 90 nm and 184
A:350 thickness of 580 nm
96 ZnCl2 + 1 M KCl 5 mM -1.0 10 min B:75 – 50 nm Si/SiO2 Cu2O/ZnO heterojunction [128]
solar cells with different
Cu2O absorber thickness

44
exhibited the highest power
conversion efficiency
of 0.52%
97 ZnCl2 + 3 M KCl 0.2 mM, pH:5 -1.0 1h B:80 80–100 n­ ITO/glass The layers of ZnO exhibited [129]
m Eg values of 3.28, 3.30,
3.31 eV for rods, disks, and
porous network.
98 Na2Zn(OH)4 + 120 g/L 5 mM 10 mV – A:300, A: 4 h – ITO The ZnO structure appears [130]
NaOH 400, to be a dominant factor that
500, 600 promotes the photocatalytic
activity through the
presence of large effective
areas for radical-organic
interactions and effective
interfacial charge transfer.
99 Zn(NO3)2.6 H2O 0.1 M/ -0.6 30 min P:100 – 357 nm (ITO)- Hall effect measurement [131]
+ 1.2 mM Na2S2O3.5 H2O pH:5.74 coated glass results confirmed that the
+ 0.1 M HCl (8–10 Ω/sqr ZnO thin films have n-type
/square conductivity with a low
electrical resistivity of
6.54 Ω cm, carrier
concentration of −1.3×1017
cm−3 and mobility of
7.35 cm2V−1s−1
100 Zn(NO3)2 + 0.1 M KCl 0.001 M -1.0 10 min A:400 A:1 h 5 µm FTO AFM study endorsed the [132]
granular structure of the
ZnO grains while by XRR
study the thickness of the
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

ZnO film was found to be

about 11 nm.
101 Cd2++2OH-→ Cd(OH)2 → 0.005, 0.01, -0.71 2700 s T:71 ± 2 – 542–798 ITO glass 0.02 M of concentration, the [133]
CdO+H2O 0.02, 0.04 nm crystallite size decreased
and 0.08 M from about 60–38 nm as the
concentration decreased
102 NO3-+H2O+ 2e-→NO2- 0.01 M, -0.71 2700 s T:72 ± 2, 385 nm ITO glass SEM images revealed that [134]
+ 2OH- pH:4,5,6,7,8 A:420 and surface morphology
B. Amudhavalli, R. Mariappan and M. Prasath

Cd2++2OH-→ Cd(OH)2 → 681 nm, depended on solution pH.

CdO+H2O 515 nm When pH was relatively low
such as 5 and 4, pyramidal
form of CdO appeared on
the surface of the films.
V. Preparation of pure and doped ZnO, CdO and CdZnO thin films using SILAR method
Sr.No. Bath composition Molarity/pH Bath Time (min)/ Preheate­ Preheated (P) Film Substrates Remarks Ref.
tem­ immersion or d (P) /Annealed thickness used
perature deposition /Anneale­ (A) time
cycles d (A)
tempera­
ture (oC)
103 ZnSO4 + 2 NaOH → 0.1 M, 90 – A:400 A:2 h 930–710 glass SEM analysis reveals the [135]
Na2ZnO2 + H2SO4 pH:9 ± 2 nm formation of flower-like
Na2ZnO2 + H2O → ZnO morphology formed by a
+ 2NaOH number of nanowires with

45
doping concentration
104 Zn(NO3)2 0.01 M 75 60, 120, 180 A:350 A:4 h FTO ZnO nanorod PEC [136]
+ 0.02 M N2H4·H2O performance can be
enhanced by decorating
(and/or doping) by noble
metal as well as by forming
composite with visible light
active semiconductor
105 ZnSO4 + 2 NaOH → 0.1 M, 90 80 A:400, A:2 h, 1 h 950–750 glass low cost grown Ag-doped [137]
Na2ZnO2 + H2SO4 0.2 M, pH:9 500 nm ZnO nanorod a good
Na2ZnO2 + H2O → ZnO candidate for high quality
+ 2NaOH vapor sensor
Dopant 1,3,5 wt% AgNO3
106 ZnSO4 + NaOH + Dopant 0.123 M, 1 M 90 200 dips A:400 A:2 h – glass Mn-ZnO film did not [138]
1,3,5 wt% MnCl2 reached an equilibrium
resistance value in its gas
response and the sensor
already reached its
detection limit at 667 ppm
for ammonia gas sensing
107 Zn(NO3)2.6 H2O + NaOH 0.1 M, 0.5 M 6000 rpm, 4 P:100 P:12 h – glass Synthesis of ZnO / Ag2O NCs [139]
cycle by depositing Ag2O
nanoparticles over ZnO NFs
through unique p-SILAR
assisted method
108 ZnCl2 + 4NH4OH→[Zn 0.1 M, pH:11 90 250 cycle A:200–4­ A:1 h 250–650 glass The crystallite size of the [140]
(NH3)4]2++4 H2O+ 2Cl-→ 00 nm films increased with
Zn2++4OH-→Zn annealing temperature
(OH)2→ZnO
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

109 Zn(NO3)2 0.1 M, 0.02 M 50 6000 rpm – – – glass pseudo successive ionic [141]
+Na2S+methanol layer adsorption and
reaction (p-SILAR) is
effectually modified for
superior deposition of metal
sulfide QDs on NPs
110 Zinc Chloride and 0.025 M, pH:9 80 15 cycle A:450 A:1 h – glass SILAR is suggested to be a [142]
aqueous ammonia good preparatory method
B. Amudhavalli, R. Mariappan and M. Prasath

for ZnO thin films.

111 ZnSO4.7 H2O + 25% 0.05 M, pH:11 95, 90 25 cycles, 50,75, A:250, A: 1 h – glass 50–100 cycles illustrated the [143]
ammonia 100 cycles 350 good optical quality.
Zn(NO3)2.6 H2O
+ ammonia
112 Zinc acetate dehydrate 0.1 M 90 50 A:400 A:1 h – glass The gas sensing study shows [144]
+Isopropanol a maximum response of the
+ Dietheanolamine films at 1000 ppm of
+ dopant (1,3,5%) ethanol was found to be
bismuth Chloride around 60% with an
operating temperature
of 400°C.
113 Zn(NO3)2 0.1 M, pH:11 50 100 A:450 A:2 h 250 nm glass the Zn1−xCuxO (x = 0.05, 0.10, [145]
+Na2S+methanol 0.15, 0.20) thin films were
+ dopant CuSO4 prepared by a simple and
facile SILAR method

46
114 Zn(NO3)2 0.1 M 20 50 A:450 A:10 min 30 nm FTO The ZnO nanorods [146]
+Na2S+methanol electrochemically deposited
CdSe/ZnO on FTO substrate were
covered with CdSe by means
of two different procedures:
successive ionic layer
adsorption and reaction
(SILAR) and electrochemical
pulse methods
115 Zn(NO3)2.6 H2O+ 25% 20 mM, pH:11 10 90 ± 2 A:200 A:1 h – FTO ZnO nanorods have been [147]
ammonia performed using successive
ionic layer adsorption and
reaction (SILAR) technique
at room temperature (27°C)
in order to form nano
heterostructure solar cells
116 Cd(NO3)2 + 2NH4OH → pH:11.5, 0.1 M – – P:200 P:60 min – glass Band gap of Zn doped CdO [148]
Cd(OH)2 (s) + 2NH+4 semiconductor thin films
+ 2NO− grown at room temperature
Cd(OH)2 (s) → CdO(s) by the SILAR method can be
+ H2O adjusted to various values
(Cd(NO3)2 + 4 H2O) by doping, demonstrating
+ (Zn(NO3)2 + 6 H2O) that these thin films can be
used as an alternative device
for photovoltaic solar cells.
117 Cd(CH3COO)2.2H2O pH:12.0, 0.1 M 20 s 80 A:350 A:1 h 545, 673, glass PEG addition can improve [149]
+ polyethylene glycol 855 and the quality of the films so
+ aqueous ammonia 1444 nm that functional solar films
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

can be produced by SILAR

deposition technique.
118 Cd(CH3COO)2·H2O 0.1 M 20 80 A:350 A:45 min – Soda lime 1.5% Ca doping, the [150]
+ doping 0.5,1.0,1.5,2.0 glass reduction in sheet
and 2.5 M% calcium resistance and parallel
ratios) CaCl2 resistance points out the
formation of a large number
B. Amudhavalli, R. Mariappan and M. Prasath

of energy levels in the

bandgap.
119 Cd(COOCH3)2.2 H2O 0.1 M 10 85 A:350 A:45 min 2.40, 1.90, glass The optical bandgap energy [151]
+ (HOCH2CH2)3 N 1.25 and was estimated based on the
0.95 µm UV–vis spectroscopies
which were obtained in the
range of 2.16–2.46 eV.
120 CdN2O6.4 H2O7 0.05 M, pH:12 20 cycle 85 A:200 A:50 min – glass The films exhibited good [152]
+ Zirconium (IV) optical properties with
OxidChlorid (at reduced bandgap energies
different dopant for the doped samples and
percentages of 0,2 good electrochemical
and 5) properties
121 Cd(NO2) 3 + 2NH4OH → pH:10.4 20 s 80 A:260 – ~ 275 nm glass High gas-sensing ability [153]
Cd(OH)2 + 2NH4NO3 for CdO-1, with 78% sensitivity in

47
Cd(OH) 2 + NH4OH → ~ 345 nm presence of 1000 ppm LPG
NH4CdO2 + H2O for CdO-2, at a relatively low operating
NH4CdO2 + H+ → CdO ~ 387 nm temperature of 260 °C
+ NH4OH for CdO-3
and ~
405 nm
for CdO-4.
122 4
Zn(NH3)2+ 0.1 M 10 min 80–100 A:450 A:2 h 320–360 glass large scale CdO-ZnO thin [154]
+ 2NaOH-→Na2Zn(OH)4 nm films as an efficient
+ 4NH3 electrode in high-
Zn(OH)2→ZnO+H2O performance gas sensing
Cd(NO3)2 and open up the further
+ 2NH4OH→Cd(OH)2 scope in selective gas sensor
+ 2NH4NO3→CdO+H2O device application
123 Cd(NO3)2.4 H2O+Na2S 0.1 M 2h 80 A:250 A:12 h 6 µm FTO glass SILAR the solution pH does [155]
0.9 H2O not need to be controlled
precisely like that in CBD
and the particles sizes are
highly reproducible.
124 ZnCl2 +NH3 →[Zn 0.1 M 10 min 80 A:400 A:1 h 250–500 glass The XRD and SEM studies [156]
(NH3)4]2++ [Cd (NH3)4]2+ nm showed that CdxZn1−xO thin
films had a polycrystalline
structure and the phase
transition occurred from
hexagonal wurtzite phase to
cubic phase with increasing
Cd concentration (x) from 0
to 1.
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

V. Preparation of pure and doped ZnO, CdO and CdZnO thin films using Chemical Vapor Deposition method
Sr.No. Bath composition Molarity Flow rate pH Growth Growth Film Substrates Remarks Ref.
Preheate­ Preheated (P) thickness used
d (P) /Annealed
/Anneale­ (A) time
d (A)
tempera­
ture
B. Amudhavalli, R. Mariappan and M. Prasath

(T) (oC)
125 0.025 g Zinc acetate 60 L/h – A:400 – 220 nm, glass high-quality ZnO films for [157]
dehydrate + 0.1 g 350 nm efficient gas sensors
methanol
126 Zn 0.1 M N2 121/min – T: T:15 min 200 nm Silica increase electrical [158]
(CH3COO)2.2 H2O+HCL 300–500 conductivity and power
factor keeping the thermal
conductivity low.
127 zinc acetate dehydrate 0.04 mM 200 ml/min – T:350, – – Glass The uniformity of the films [159]
+ 2-hydroxo-1- 400, 450 and the average crystallite
naphthaldehyde, size of the particles in the
+ tetrahydrofuran (THF) film decreases with
increasing temperature.
128 Zn (CH3COO)2.2 H2O 0.5 g 1.5 L/min – T:400 T: 30 ± 5 min 100–2150 Silica Nb doped ZnO films [160]
+ Nb (OCH2CH3)5 nm produced from AACVD
+ methanol + Toluene generally showed a

48
crystalline nature with a c-
axis preferential orientation
along the 0 0 2 plane,
although at higher
concentrations the films
showed amorphous
behavior.
129 Zn powder – – – T: 575 T:10 min – α-Al2O3 PL spectra from the [161]
and 725 substrates undoped and as-grown N-
doped films were composed
of the GB emission at
~530 nm and the NBE
emission with the two peaks
denoted by α (~376 nm) and
β (~386 nm).
130 25–75 mg zinc-acetate- – 80 L/h – T:350, A:1 h 20–80 nm FTO glass Best power conversion [162]
dihydrate + 10 ml A:500 efficiency (PCE) of 11.75%
methanol
131 ZnO powder + 4.0 wt% – 40 sccm, – T:550–9­ T:15 min 200 nm glass All the X-ray diffraction [163]
Ga2O3 400 sccm 25 patterns of the ZnO/GZO
films were dominated by a
ZnO(002) peak, indicating
the successful growth of
highly c-axis oriented films
132 ZnO + Tm2O3 + Yb2O3 – 0.74 μmol/s. – T:500–7­ T:30 min 175 nm − c-plane Improved crystal quality of [164]
00 500 nm sapphire the ZnO host by utilizing the
(0001) NW configuration.
substrates
133 CdO powder – 1.5 L/min – T:2 h [165]
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

T:550–8­ 0.44–2.0­ c- or r- Temperature dependent

50 1 µm plane Hall effect measurements
sapphire were performed for the
substrates undoped CdO films with
carrier concentrations (n)
ranging from 2.4 × 1019 to
2.0 × 1020 cm−3
134 CdO powder Pressur­ 2–10 L/min – T:150–4­ – 100 nm glass Optical bandgap decreased [166]
B. Amudhavalli, R. Mariappan and M. Prasath

e:5–90 Torr 50 from 3.10 to 2.35 eV with

increasing deposition
temperature
135 Tertiary butanol – – 282–46 – T:330 200 nm glass HRXRD peak shift direction [167]
C4H10O (TBA) μmol/min as a signature of a lower Zn
+ dimethylcadmium – and content into the cubic
C2H6Cd (DMCd) 225–2760 s phase. Wurtzite Zn1−xCdxO
+ diethylzinc –(C2H5)2 coexists with the
Zn (DEZn) polycrystalline cubic phase
of the alloy at 24.1% and 30%
Zn contents
VI. Preparation of pure and doped ZnO, CdO and CdZnO thin films using Atomic Layer Deposition method
Sr.No. Bath composition Molarity / pH Pulsing Deposition cycle Anneali­ Annealing (A) Film Substrates Remarks Ref.
time ng (A)/ /Deposition thickness used
Depositi­ time
on

49
tempera­
ture
(T) (oC)
136 ZnO – – – T:200 – 15, 38, n-Si(100) The phonon contribution to [168]
110, substrate total thermal conductivity
118 nm dominates over the electron
thermal conductivity.
137 ZNo (Diethylzinc – – – T:150 – 3–9 nm p-Si(100) Sub-channel forms at the [169]
(DEZ)+H2O) substrate interface between the two
ZnO (Diethylzinc channels that improves not
(DEZ)+O3) only the mobility but also
the bias stability.
138 Diethylzinc (DEZ)+H2O2 – – 100,200,400,80­ T-80 – 632.8 nm Silicon The oxygen vacancy [170]
0,1200,1600 decrease was due to the
reduced grain boundaries
and improved crystallinity
resulting from the film
thickness increase,
consequently weakening
the resistivity through a
large decrease in carrier
concentration and a small
increase in carrier mobility.
139 diethylzinc [DEZ, Zn – 0, 1,3,5 s 500 T:100, – 72.6,84.2­ Si(100) Dominance of (002) [171]
(C2 H5)2] 150,180,­ ,91.1103.6 wafer orientation in the presence
200 nmg of oxygen during the ALD
growth process.
140 Diethyl zinc (DEZ) 0.1, 3, 5 s 220–2200 T:80 400–1700 8-inch ZnO-PMMA [172]
+ (ZnAc2⋅2 H2O) nm (100)- nanocomposites can be
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

+ (NaOH)+ Methylene oriented easily synthetized and used

blue (MB) + Sodium silicon in wastewater treatment,
lauryl sulfate (SDS) wafers but also in devices such as
sensors, photovoltaics and
optoelectronics.
141 Diethylzinc (DEZ)+H2O – 2s 50,100,200 T:150, A:3 h 8.7, 17.4, Si wafer The 180-min flashing of a [173]
A:700 34.8 nm red LED powered by ZnO
NMs supercapacitors
B. Amudhavalli, R. Mariappan and M. Prasath

suggests great potentials of

NMs electrodes in practical
applications.
142 Diethyl zinc (DEZ) and – 0.2–10 s – T:100 – 30 nm FTO glass The results suggested that [174]
Trimethylaluminum AZO IOS prepared by ALD
(TMA)+ dopant Al2O3 also has the potential to
enhance the
photoelectrochemical
efficiency by combining
with other similar films.
143 Diethylzinc (Zn(C2H5)2, – 5 s, 30 s 300 cycle/ZnO, T:200, A:2 h 28,29,32 Si substrate Initial discharge capacity [175]
DEZn) + dopant 500 cycle/SnO2 A:1000 nm 1795 mAh g−1 and 588 mAh
(Dimethylamino tin (IV) g−1 after 100 cycles at
(Sn [(CH3)2N]4, 50 mA g−1
TDMASn)
80 x(2ZnO+3SnO2)

50
80 x (20ZnO+30SnO2)
144 Diethyl zinc (DEZ, – 1 s, 50 s 100, 400, 800 T:50, – 20, 98, glass Minimum ZnO film [176]
Zn(C2H5)2,+ H2O 150, 250 100, thickness of 50 nm was
138 nm needed to maximize
photocatalytic activity, and
the highest photocatalytic
activity was obtained at a
nanograin size of 20 nm and
a (002)/(101) ratio of 2.2.
145 Diethylzinc (DEZ) + H2O – 4 s, 5 s 100,500,600 T:150,20­ – 18,90,108 glass Very good transparency was [177]
0,350 nm obtained at the cost of
16,80,96 quality of the deposited
nm thin film
4,20,24 n­
m
146 Poly (methyl – 1 s, 120 s 150 T:35 – 32 nm, polished Application in flexible [178]
methacrylate) (PMMA), 80 nm silicon electronics and nanoscale
Diethyl zinc (DEZn, Zn substrates optoelectronic device
(C2H5)2 +H2O (Si (100)
147 diethyl-zinc (DEZ), and 3 s,4 s 0.08, 0.1 nm per T:200, A:5 min 60 nm, GaN The ZnO films prepared at [179]
hexakis +dopant cycle 300 70 nm substrate 300 °C on GaN substrates
(dimethylamino) A:400,80­ are epitaxial, but the Ga
gallium (C12H36Ga2N6) 0 doping deteriorates the
crystallinity
148 Diethyl zinc [Zn(C2H5)2; – 1,1,4 s 25,20,15 T:155–2­ – 230 nm glass The ZnO and AZO thin films [180]
DEZ] + H2O + dopant 00 were polycrystalline, with
Trimethylaluminum [Al the AZO films crystallizing
(CH3)3; TMA], preferentially in the (1010)
direction.
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

149 Diethyl zinc [Zn(C2H5)2; – 5s 50, 1000 T:180 – 20 nm n-type The accurate control on the [181]
DEZ] + H2O, dopant silicon (111) deposition of thin films
1,3,5% substrates makes this process a
Trimethylaluminum suitable method to be used
(TMA) in the optoelectronic
industry as a precise coating
technique with attenuation
applications.
B. Amudhavalli, R. Mariappan and M. Prasath

150 Diethylzinc + H2O – 1 s, 3 s 100 T:150 – 2.5–10 n­ glass ZnO shells on Agmetal cores [182]
m increase the intensity of
light around NPs, allowing
the plasmonic cores to fully
utilize incident light.
151 Diethylzinc (DEZ) – 1s 100, 150, 170 T:130 − 1­ – 12–27 nm Silicon Future use of ALD in all [183]
+ 0.45 µm Poly 80 substrate organic electronic devices
(Tetrafluoroethylene) not only on substrates, but
(PTFE) more importantly directly
onto the organic active
layers.
152 Diethylzinc (DEZ) + H2O – – – T:25–250­ – 1.5–2 nm single side ZnO layers deposited at [184]
nm polished c- different temperatures,
Si (100) giving additional insights on
substrates the material properties
deposited by PE-ALD

51
153 Diethylzinc (DEZ) + H2O – 10 s, 1 s 100 T:60,80,1­ – 8–200 nm p-type Si The effective activation [185]
00,125,1­ (100) energy was evaluated from
50,200 wafers the effective rate constants
of temperatures, which was
found to be ~8.50 kJ/mol.
154 Diethylzinc (DEZ) + H2O – 5 s,1 s 125 T:125 – 100 nm SiO2/Si Transfer between ZnO and [186]
substrate MoS2 surface and the re-
absorption of light photon
resulting in the production
of electron-hole pairs.
155 Diethylzinc 0.1 s, 10 s – T = 150–­ – 150 nm glass An increase in the carrier [187]
+ Trimethylgallium 200 concentration widened the
+H2O optical bandgap of ZnO thin
films by the Moss-Burstein
effect.
156 Diethylzinc (DEZ) + H2O – 5s 20, 130, 150 T:130, – 20 nm Silicon Dual-layer channel TFTs can [188]
200 wafer be a promising candidate for
the application in large area
flat panel displays
157 DEZ (0.1 s)→N2 (10 s) → – 0.1 s, 108 nm/cycle, T:60–200 – – SiO2/Si XRD and SEM results [189]
H2O / H2O2 (0.1 s)→N2 10 s, 0.1 s 0.88 nm/cycle, substrate indicated that using H2O2
(10 s) 0.21 nm/cycle, instead of H2O provides an
0.18 nm/cycle, O-rich condition for the
0.27 nm/cycle growth of ZnO film
158 Diethylzinc (DEZ) + H2O – – 50,70,135,167,20­ T:200` – 69.2,71.9­ Silicon The analysis of wide spectral [190]
0,360,460 ,71.3,76.0­ wafer range SE provides access to
,68.2,67.­ phonon modes, the band
2,68.4,69­ gap, and electrical transport
.8 nm
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

properties for these TCO

thin films.
159 0.2 s Diethyl zinc [Zn – 0.2 s, 0.75 s – T:200 – 20 nm, fused ZnO thin films prepared in [191]
(C2H5)2; DEZ] + 0.2 H2O 70 nm quartz this manner may serve as a
+ 0.75 s N2 (SiO2) key component in the
B. Amudhavalli, R. Mariappan and M. Prasath

substrates design and fabrication of

short wavelength light-
emitting devices
160 0.2 s Diethyl zinc [Zn – 40 s, 60 s 0.2 nm/cycle T:100 – 20 nm, Si wafer Present method may find [192]
(C2H5)2; DEZ] + 2 s H2O 100, 250 50 nm many applications in array
+ 0.75 s N2, sodium devices such as field-effect
dodecyl sulfate, transistors, sensors,
Hydrofluoric acid electrodes, and two-
dimensional photonic
crystals
161 13 ms ZnEt2 + 20 ms H2O – 30 s, 20 s 0.07 nm/ T:60,65,7­ – 10 nm/ ITO glass ZnO have been developed [193]
PEDOT:PSS, Cesium cycle, 150 0,75 ZnO, and employed as interface
bromide, Lead bromide layers for energy level
matching and electron
transport in order to achieve

52
high performance
perovskites based
optoelectronic devices.
162 0.2 s Diethyl zinc [Zn – 5s 480 T:200 – 51.4–65.8 polished Si ALD-derived AZO films from [194]
(C2H5)2; DEZ] + 2 s H2O nm (100) with TMA and AIP sources exhibit
+ 0.1 s N2 +dopant AlCl3 native oxide promising prospects as TCO
and quartz/ electrodes for applications
borosilicate in optoelectronic devices.
glass
substrates
163 0.2 s Diethyl zinc [Zn 2 s,1 s 100 T:100–2­ – 20–50 nm Si wafer, The EQY of bulk-ZnO was [195]
(C2H5)2; DEZ] + 0.1 s H2O 50 Quartz glass found to be ~18-times
+ 0.1 s N2 higher than for ALD-ZnO
and the lifetime of the
interband transition (UV-
peak) was found to be at
least ~14-times faster
164 0.2 s Diethyl zinc [Zn 2 s, 10 s 200, 350, 500, T:200, A:2 h 30,50,70,­ Glass, ITO FF-controlled ZnO-based [196]
(C2H5)2; DEZ] 600, 700 A:200 85, NW structures efficiently
+ 0.2 s H2O + 10 s N2 100 nm trapped light and would be
highly suitable as light
polarizers in many
optoelectronic devices.
165 Dimethylcadmium 2 s, 10 s 100 T:150 T:1 h 2 nm Si substrate ALD system and no [197]
+ H2O noticeable impurities are
detected via XPS
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

VII. Preparation of pure and doped ZnO, CdO and CdZnO thin films using Pulsed Laser Deposition method
Sr.No. Bath composition Basic Working Power Density/ Preheate­ Preheated (P) Film Substrates Remarks Ref.
Pressure (P) / pressure Pulse Energy d (P) /Annealed (A)/ thickness used
target (P) / target /Anneale­ deposition
substance rotation d (A)/ time
distance (D) speed (S)/ deposi­
Frequency tion
tempera­
B. Amudhavalli, R. Mariappan and M. Prasath

ture
(T) (oC)
166 Zinc nitrate tetrahydrate P:50 m Torr to – – T:300 T:45 – Silicon The concentration of defects [198]
+ dopant Europium 250 m Torr was high in the case of the
nitrate pentahydrate powder, so it has shown
very small NBE with higher
defect (DLE) and Eu3+
emission.
167 ZnO +dopant Al2O3, D:50 mm S:10 rpm D:5 J/cm2 T = 500 – 300 nm c-plane The X-ray photoelectron [199]
Sb2O5 P: 6.66 × 10−4 P: sapphire spectroscopy analysis
Pa 0.13–66.66 substrate exhibited that the thin films
Pa, contained more Sb5+ than
Sb3+; therefore, the p-type
conduction was owing to
the Sb5+ ions, which formed
the SbZn–2 VZn complex.

53
168 ZnO + dopant V2O5 P:2×10−3 Pa F:5 Hz D:2 J/cm2 T:500 – 400–600 boro- Optimization of the [200]
D:40 mm nm alumino- substrate temperature as
silicate well as the oxygen partial
glass pressure during the film
deposition is necessary for
further improvements of the
resistivity of the PLD
VZO films.
169 ZnO P:10−4 Pa F:2 Hz E:300 mJ T:600, 100 nm, glass O-polar and Zn-polar ZnO [201]
A:900 300 nm films were grown on c-
sapphire by pulsed laser
deposition.
170 ZnO +Co3O4 D:8 cm – D:4.2 J/cm2 T:500, A:2 h 170–210 sapphire Pulsed nanosecond laser [202]
P: P:4×10−5 A:100 nm substrate radiation induces the
Torr formation of center-
oriented cone-shaped
structures and micro-
hiskers on the target surface
171 98% ZnO + 2 wt% Al2O3 D:2.5 cm F:10 Hz D:2 J/cm2 T: T:45 min – Silicon (p-Si The deposited samples with [203]
P: 2.6, 5.3, room 100) and presence of nano /
10.6, temp. glass microstructure and Zn
133.3 Pa exhibited low transmittance
as compared to the films
deposited in O2 or low
pressure He.
172 ZnO:Eu3+ P: 3×10−5 P: – T:300 – 115 nm Intrinsic- XPS high resolution spectra [204]
mbar 0.133 mbar type Si of the O 1 s peak confirmed
(100) the creation of new defects
substrate during electron beam In
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

general, ZnO:Eu3+ films

show potential for
applications as a source of
red light in optoelectronic
devices.
173 ZnO power +Ge Power P: 2.0×10−5 Pa P: D:2 J/cm2 T:25–500 T:45 min, 95 nm Soda lime This work provides valuable [205]
0.5–2.5 Pa. 90 min glass information and new insight
for fabricating high
B. Amudhavalli, R. Mariappan and M. Prasath

performance TCO materials.

174 ZnO:Cu (2 wt%) P: 2×10−6 F:10 Hz D:2.5 J/cm2 T:: – 60 ± 2 n­ p-Si (100) Fabricating Cu-doped ZnO- [206]
mbar room m substrates based photodetectors with
temp. low operating voltages and
their excellent stability
175 0, 1, 2, 3, 4 and 5 wt% Sm D:8 cm F:1 kHz – T:25 T:1 h – borosilicate All films are suitable for use [207]
+ ZnO P:10−5 Torr glass in optical devices for UV and
substrates blue emission.
176 Zinc oxide + gold D:5.2, 6.5 cm P:0.67 Pa D: 4.5, T:400 T:20 min 20–475 n­ Si (100) The final thickness of the [208]
F:10 Hz 13.6,20.9 J/cm2 m wafer films was closer to the sum
substrates of the accumulation rates of
ZnO and Au, and greater
than the sum of the
individual deposition rates.
177 Zinc oxide +A2O3 D:35 mm – D:0.8,0.84, 1.0, T: T:10 min 150 nm (100) single AZO nanocomposite films [209]
2.4 J/cm2 room crystal are expected to be used in

54
temp. substrate real applications such as
thin film modules deposited
on flexible polymer
substrates for ubiquitous
harvesting of the
waste heat.
178 ZnO +MgO P:10−4 Pa F:2 Hz – T:600 T:10 min > 0.5–5 ITO ZnO containing [210]
P:100 P:2 h nm optoelectronic devices,
while Zn-terminated
surfaces could be of interest
for photocatalytic and
sensing applications.
179 ZnO + ml-MoS2 P:1 Pa F: 5 Hz D: 100, 300 mJ T:200, – 400 nm Single-side Simple and efficient method [211]
650 polished to grow continuous large-
Al2O3 area ZnO/MoS2 hetero-
(0001) structures is demonstrated
substrate by pulsed laser deposition
180 ZnO P: 10−8 F:15 Hz D:40 mJ T: – 10 nm glass ZnO structure with the [212]
− 5×10−6 Room and largest peak corresponding
mbar, temp. 220 nm to (002) orientation but
D:50 mm some films contain Zn with
(101) orientation
181 n-ZnO/p-Si D:50 nm, P: F:10 Hz D:45 mJ T: – 200 nm p-type Si The photovoltaic (PV) [213]
1×10−6 mbar Room (100) property of n-ZnO/p-Si
temp substrate heterojunction was
investigated by using
current-voltage (J-V)
measurement under
illumination at 70 mW/cm2.
(continued on next page)
Journal of Alloys and Compounds 925 (2022) 166511
 Table 2 (continued)

I. Preparation of pure and doped ZnO, CdO and CdZnO thin films using chemical bath deposition method

Sr.No. Bath composition Deposition Deposition Annealing Annealing pH Film Substrates Remarks Ref.
temperature time temperature (oK) time thickness used

182 Eu2O3:ZnO P:5×10−5 Pa P:10 Pa D:2 J/cm2 T: Room – 320, Silica XPS revealed the ratio of Eu [214]
D:50 mm temp. 370 nm substrate divalent and trivalent states
and 300 as 35%:65% and 27%:73% for
sample deposited at room
temperature and 300 °C.
183 AZO/n-ZnO/p-Si – P: D: 5.2 J/cm2 T: Room T:15 min 200 nm p-Si Al doped ZnO (AZO) layer [215]
5.3–9.3 Pa temp. to substrates was more improved by post
350, annealing at 200 °C, so that
B. Amudhavalli, R. Mariappan and M. Prasath

A:200 the heterojunction with and

without AZO layer showed
power conversion efficiency
(PCE) of 0.61% and 1.5%,
184 Zinc dust target (Zn) P:5×10−5 Pa P:10 Pa D:2 J/cm2 T:450 T:30 min – Quartz Films have crystalline [216]
and Cadmium sheet D:50 mm substrate structure, high homogenous
(Cd), 4-nitrophenol (4- surface, and nano structural
NP), Sodium particle size formation
borohydride (NaBH4)
185 Copper target P:10−4 Tarr F:10 Hz, Power:10 W – T:30 min 712, Si substrate XRD scan shows an increase [217]
+ Cadmium sheet D:50 cm 745 nm in the intensity of (111) and
+ 4-Nitrophenol decreasing in (200) peak
(4-NP)+ Sodium confirming the growth of
borohydride (NaBH4) doping of CuO through CdO
thin film
186 Cadmium oxide target P:20–100 F:1 Hz D:2 J/cm2 T:500 – – Si substrate CdO Undoped, thin films [218]

55
mbarr were deposited on the
substrates of Si using a laser
Nd: YAG Reactive pulsed
deposition technique
187 CdO+Doping (1–11%) Sn P:5×10−7 Tarr F:2 Hz D:300 mJ T:750 – 500 nm MgO (111) The band gap increases with [219]
substrates doping and reaches a
maximum of 2.87 eV when
the doping level is 6.2%.
188 CdO Target P:5×10−4 Pa P:6 MPa D:25 J/cm2 A:800, T:6 h 450, 300, glass TEM observation showed [220]
F:10 Hz 900 250,200, that more crystalline defects
170 nm like lattice distortion,
dislocation and amorphous
structure existed in the
small grained (25 nm)
CdO film
189 CdO + SnO2 1.0×10−6 N/m2 F:10 Hz Growth T:Room – 100 nm Quartz Highly conducting and [221]
rate:3 nm/min temp., substrate transparent tin-doped CdO
150, thin films grown via pulsed
300,450, laser deposition could be an
600 excellent candidate for
future optoelectronic
applications.
190 CdO + ZnO Powder 5×10−6 Torr F:10 Hz – T:200,25­ – 300–400 2947 glass Highly suitable as an active [222]
0,300,40­ nm substrates layer in CdZnO/ZnO
0,500 heterostructures meant for
optoelectronic applications.
Journal of Alloys and Compounds 925 (2022) 166511
B. Amudhavalli, R. Mariappan and M. Prasath
is when the material contains oxygen and one metallic element that
is in two or more oxidation states within the lattice [223].
There are many different properties associated with complex
oxide materials, including ferromagnetism, ferroelectricity, piezo­
electricity, and high-temperature superconductivity. But these
properties are not restricted to just complex oxides, yet at least one
is exhibited by all complex oxide materials. These properties are
often exhibited because the electrons within the d and f orbitals are
strongly correlated, and this means that each electron has an in­
dividual influence on the neighboring electrons. This electronic ar­
rangement causes the materials to be a hybrid electronic structure
that lies between ionic and free-electron materials [224–226].
ZnO based thermoelectric materials are emphasized, due to the
merits of inexpensiveness, earth abundance, chemical and high
temperature stability as well as nontoxicity. A few examples of ZnO,
CdO and CdZnO related oxide systems are briefly reviewed and
proposed as useful model systems to investigate and understand the
correlations between chemical compositions, phase equilibrium,
microstructure surface morphology, optical and electrical proper­
ties [227].
Complex oxides are multifunctional materials that could even­
tually lead to energy-efficient, advanced electronic memory com­
ponents and quantum computing devices. Our findings are a strong
proof of the rising importance of complex oxides, which could be
ready to go for future microelectronic applications.
5. Conclusions
Zinc oxide (ZnO), cadmium oxide (CdO) and cadmium zinc oxide
(CdZnO) thin films have played a very important role in the present
modern scientific technology. We have presented a recent review on
ZnO, CdO, and CdZnO thin films using different deposition methods
with optimised deposition parameters for the preparation of device
quality thin films. Chemical methods have many advantages and are
widely used as thin film deposition methods because they are re­
latively cheap, convenient for large area deposition, and have good
tuning capability by adjusting and controlling the thin film deposi­
tion parameters systematically. Therefore, ZnO, CdO, and CdZnO thin
films are very interesting for various industrial and modern tech­
nological applications such as gas sensors, solar cell transparent
contact fabrications, surface acoustic wave systems, high perfor­
mance thin film transistors, organic light emitting devices, wireless
communications, telecommunications, integrated circuits, rectifiers,
photoconductors, light crystal displays, lithography, micro-electro­
mechanical systems, etc., where large area is desirable.
Data Availability
Data will be made available on request.
Declaration of Competing Interest
The authors declare the following financial interests/personal
relationships which may be considered as potential competing in­
terests: Dr. R. Mariappan reports financial support was provided by
Adhiyamaan College of Engineering. Dr. R. Mariappan reports a re­
lationship with Adhiyamaan College of Engineering that includes:
employment and funding grants.
Acknowledgments
The authors are very much grateful to the Periyar University PG
Extension Centre, Dharmapuri and the University Grants
Commission-South Eastern Regional Office (UGC-SERO), Hyderabad
(India), for financial support under the project (No. MRP-4892/14
56
Journal of Alloys and Compounds 925 (2022) 166511
(SERO/UGC)) and Adhiyamaan College of Engineering (Autonomous),
Hosur, Krishnagiri.
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