Materials Science in Semiconductor Processing 121 (2021) 105361

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Materials Science in Semiconductor Processing

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Synthesis and characterization of gallium oxide in strong reducing growth

ambient by chemical vapor deposition
P.R. Jubu a, b, *, F.K. Yam a, **, O.S. Obaseki a, c, Yushamdan Yusof a
a
School of Physics, Universiti Sains Malaysia (USM), 11800, Pulau, Penang, Malaysia
b
Department of Physics, University of Agriculture Makurdi, P. M. B. 2373, Makurdi, Benue State, Nigeria
c
Department of Physical Sciences, Landmark University, Omu-Aran, Kwara State, PMB 1001, Nigeria

A R T I C L E I N F O A B S T R A C T

Keywords: Deposition of gallium oxide (Ga2O3) from oxide powder precursor by using the high-temperature chemical vapor
Gallium oxide deposition technique (CVD) has often eluded amorphous soda lime glass substrate because of its tendency to
Amorphous soda lime glass substrate deform at high temperatures. Herein, Ga2O3/glass films have been systematically synthesized by the CVD route
Chemical vapor deposition
in the temperature range 850–1000 ◦ C without deformation to the substrates. X-ray diffraction revealed Ga2O3
Crystal structure
α-β bi-phase with increasing crystalline quality and crystallite size due to rising deposition temperature. Field
emission scanning electron microscopy results showed surfaces having facetted aggregates and increasing film
thickness with rising temperature. Energy dispersive X-ray spectroscopy revealed increasing Ga and decreasing O
contents with rising deposition temperature.

1. Introduction (high-temperature) CVD. These synthesis technologies use gallium pre­

Many applications of nanoscale materials in devices require tem­
plates called substrates onto which films of materials are deposited. The
choice of suitable substrates for nanomaterials growth is dependent on
many parameters including the desired synthesis temperature and
method, lattice parameters of the nanomaterial and substrate, proposed
working environment of the nanodevice and desired surface conduc­
tivity. Among the various substrates, amorphous soda lime glass sub­
strate (AGS) is the most cost-friendly, readily available and widely
deployed growth template.
Ga2O3 is a semiconductor material with five polymorphs designated
as α-, β-, γ-, δ- and ε-phase, among which β-Ga2O3 is the best-
characterized phase [1–3]. β-Ga2O3 has received considerable interest
due to its outstanding properties such as wide bandgap (̃ 4.9 eV), high
theoretical breakdown field (8 MV/cm2), thermal stability, and chemi­
cal stability. Ga2O3 films produced on AGS have been applied in
chemical sensing [4], photoelectrolysis [5], photodetection [6,7], power
devices [8,9] and phosphors [10]. However, the Ga2O3 nanomaterials
grown on AGS are synthesized by methods including atomic layer
deposition (ALD), solution method and spray pyrolysis, which operate
optimally at temperatures lower than the oxide powder-source
cursors that require lower evaporation temperatures such as trime­
thylgallium (TMGa), triethylgallium (TEGa), gallium (III) chloride
(GaCl3), gallium nitrate hydrate (Ga(NO3)3⋅9H2O, gallium isopropoxide
(C9H21GaO3), gallium acetyl-acetonate (Ga (acac)3), trishexa­
fluoroacetylacetonate (Ga (hfac)3) and gallium amide [Ga-(NMe2)3]2 [6,
11–14].
Nieminen et al. [15] produced Ga2O3 thin films on AGS at 130 ◦ C by
the atomic layer epitaxy (ALE) method by using Ga (acac)3 precursor.
Binion et al. [4] on the other hand prepared Ga2O3 films on AGS by
atmospheric pressure CVD (APCVD) using GaCl3 as the source material
at different deposition temperatures (350–600 ◦ C). Meanwhile, Basharat
et al. in 2008 fabricated Ga2O3 nanomaterial on AGS at temperatures
50–75 ◦ C by the aerosol-assisted CVD (AACVD) using gallium amide
[Ga- (NMe2)3]2 precursor [11]. In the same year (2008), Shinohara et al.
[16] deposited Ga2O3 films on AGS by the mist CVD (MCVD) technique
using (Ga (acac)3) source. Marwoto et al. in 2012 [17] developed Ga2O3
thin films on AGS at 600 ◦ C by the direct-current (DC) magnetron
sputtering from Ga2O3 powder. In the following year (2013), Dakhel
et al. [18] used Ga2O3 powder to synthesize Ga2O3 on AGS at 600 ◦ C by
deploying the thermal evaporating technique.
Ga2O3 nanomaterials have also been deposited on sapphire at

* Corresponding author. School of Physics, Universiti Sains Malaysia (USM), 11800 Pulau, Penang, Malaysia.
** Corresponding author.
E-mail addresses: jubu_raphael@yahoo.com (P.R. Jubu), yamfk@usm.my (F.K. Yam).

https://doi.org/10.1016/j.mssp.2020.105361
Received 21 April 2020; Received in revised form 17 July 2020; Accepted 27 July 2020
Available online 17 August 2020
1369-8001/© 2020 Elsevier Ltd. All rights reserved.
P.R. Jubu et al. Materials Science in Semiconductor Processing 121 (2021) 105361

temperatures between 450 and 600 ◦ C by the metal-organic CVD undergoing deformation, due to its low strain point 500 ◦ C and softening
(MOCVD) method using TEGa source [19,20]. Kim et al. [12] also point 700 ◦ C [28]. The major factor that constitutes hindrance to the use
fabricated Ga2O3 films on Si substrates by the same synthesis technol­ of AGS in oxide powder-source and gallium metal-source CVDs has been
ogy, MOCVD, by reacting TMGa between 500 and 600 ◦ C. In 2019, the location of the substrate being too close to the source boat where
Koyama et al. [21] synthesized Ga2O3 semiconductor nanomaterial on temperature is very high (see source-substrate distance in Table 1).
3C–SiC templates from Ga (acac)3 at 350 ◦ C by the MCVD technique, Similar to our work, although with a different semiconductor material,
while Li et al. [22] produced Ga2O3 films on sapphire at 1150 ◦ C from Fadzil et al. [29] effectively deposited ZnO films on AGS from Zn powder
TMGa by the MOCVD method. Recently, Ghadi et al. [23] deposited by using TCVD system comprising two horizontal furnaces, so that the
Ga2O3 on Sn doped (010) EFG (edge-defined film fed grown) substrates precursor was placed in the first furnace with temperature varied from
at 800 ◦ C by the MOCVD method using TEGa source; while Cheah et al. 650 to 850 ◦ C, while the substrate was located in the second furnace
[24] produced Ga2O3 thin films on fused silica substrates at room tem­ where temperature was maintained at 500 ◦ C. This method is appre­
perature by spin coating method from (C9H21GaO3), followed by ciable but quite expensive, stressful, and power consuming. Our method
annealing between 500 and 900 ◦ C. In the same vein, Xu et al. [9] which uses one horizontal furnace is cheap and easy.
fabricated Ga2O3 on clean silicon substrates by spin coating using In this work, we report the synthesis of Ga2O3 films on AGS by the
GaN3O9.xH2O and subsequent annealing at 350 ◦ C or 250 ◦ C, respec­ high-temperature RA-CVD. The use of AGS as the growth template in the
tively. So far, we are not aware of Ga2O3 films produced on AGS from the oxide powder-source CVD was made possible by placing the precursor in
oxide powder-source by using the high-temperature CVD method. the high-temperature zone and locating the substrate in the far down­
Table 1 is a summary of the non-MOCVD and non-MCVD techniques stream zone where temperature was suitable for AGS. We believe that
employed by researchers to grow Ga2O3 films on various substrates by this report will promote the growth of Ga2O3 films and other semi­
using the oxide powder-source and metallic gallium-source CVDs. These conductor nanomaterials on AGS by the high-temperature CVD tech­
CVDs make use of reducing gases such as H2 gas or CO (from charcoal) to nique using oxide powder sources.
evaporate the powder source at high temperature under a technology
known as reducing-ambient CVD (RA-CVD). When evaporating gallium 2. Experimental
metal in CVD under atmospheric pressure, the technology is called
APCVD. Meanwhile, when Ga2O3 film is produced from either gallium Ga2O3 nanostructures (NSs) were deposited on AGS by the CVD
(III) oxide powder or gallium metal source without reducing gas, the method. Prior to synthesis, microscope glass slides (76 × 26 mm) made
technology is known as low-pressure CVD (LPVD). On the other hand, of soda lime glass 1 mm thick were cut into small pieces (10 × 10 mm) as
when evaporating gallium metal alone or a mixture of Ga2O3 powder substrates. The glass substrates were ultrasonically cleaned with acetone
and gallium metal or another material, the technology is referred to as at 50 ◦ C for 10 min, followed by an immersion in methanol for 5 min.
thermal CVD (TCVD). Other semiconductor materials such as ZnO and The substrates were then rinsed in deionized water and after, dried with
In2O3 are also grown from their oxide powder or metallic sources the use of synthetic air. To identify the suitable temperature region in
[25–27]. Nevertheless, as already mentioned, the synthesis of Ga2O3 the reactor where films can be successfully grown without deformation
films on AGS from Ga2O3 powder source by the high-temperature CVD to the template, four substrates were placed in separate ceramic boats
method is rarely available in the literature (see Table 1). This is probably and located at the 10, 15, 20 and 25 cm marks, respectively from the
due to the inability of AGS to withstand high temperatures without center zone (source position) of the horizontal furnace. The temperature
of the reactor was raised from room temperature (RT) to the highest
point (1000 ◦ C) and sustained for 120 min, after which it was shut down
Table 1 and allowed to cool down to RT. Observation showed that only the
Summary of CVD types for the synthesis of Ga2O3 films using non-metal-organic substrate located at the 25 cm mark could come out without deforma­
and non-chloride Ga sources, substrates, deposition temperature and source-to- tion. The 25 cm separation from the high-temperature zone was then
substrate distances. marked as the effective substrate location for the synthesis. About 58 mg
CVD Ga Atmosphere Substrate T (◦ C) X Reference Ga2O3 powder (99.998% purity) was placed in a ceramic boat and
type source (cm) loaded to the center zone of the horizontal furnace, while the glass
HRA- Ga2O3 N2/H2 Si 850- 22, [30, 31] substrate was positioned at the 25 cm separation in the far downstream
CVD 1000, 23 zone. The system was flushed with flowing N2 gas for 5 min, then the
1000
temperature of the furnace was ramped from RT to 850 ◦ C. N2 flow was
HRA- Ga2O3 Ar/H2 Si, Cu – <10 [32]
CVD stopped and 100 sccm H2 gas was then fed into the system. The process
CHA- Ga2O3 Ar/O2, CO, Si 960 2–5 [33] was allowed to last for 120 min after which the furnace was shut down
CVD H2, N2 and allowed to cool to RT. A milky film was observed on the substrate.
LPCVD mGa Ar/O2 Sapphire 900 <10 [34] The experiment was repeated for deposition temperatures of 900, 950,
LPCVD Ga2O3 Ar/O2 Si 1000, 2, 10 [35, 36]
950
and 1000 ◦ C respectively. The experimental setup for the synthesis is
LPCVD mGa, Ar/O2 Si 650 0.5 [37] shown in Fig. 1.
CaF2 Crystal structure and surface morphology were characterized using
LPCVD mGa Ar/O2, H2 Si, GaAs 900, 15 [38, 39] high-resolution X-ray diffraction (HR-XRD) PAnalytical X’Pert Pro and
700-
field-emission scanning electron microscope (FE-SEM) FEI Nova Nano­
1000
C-CVD Ga2O3 Ar/O2, CO Si, Quartz 1000, <10 [40–42] SEM 450, respectively. Film thickness was taken by cross-section
1180 method using FE-SEM. Composition was measured using energy
C-CVD Ga2O3 Ar, CO Si, 1150, <10 [43, 44] dispersive X-ray spectroscopy (EDX) attached to the FE-SEM.
Sapphire 1100
TCVD mGa Ar, He/O2 Si 900, 0.5 [45, 46]
950
3. Results and discussion
TCVD Ga, – Al2O3 1100 0.02 [47]
Ga2O3, 3.1. Crystal structure
TCVD mGa Ar/O2 Al2O3 1000 0.2 [48]

Notes: T: temperature; X: source-substrate distance; mGa: metallic gallium; The phase compositions of the samples were determined by XRD
HRA-CVD: hydrogen reducing-ambient CVD; C-CVD: carbothermal CVD; CHA- analysis. Fig. 2(a) shows XRD patterns of the prepared Ga2O3 films. Two
CVD: carbon-hydrogen ambient CVD. phases of Ga2O3 could be identified. All diffraction planes could be

2
P.R. Jubu et al.
Fig. 1. Experimental setup for the typical CVD system. The sketched T-x graph
illustrates temperature drop along the fabrication line, where T1 and xSour. are
source temperature and position, T2 is the substrate temperature, xSubs is the
substrate distance from source and x2 is a position in the upstream region.
indexed to monoclinic (β-phase) Ga2O3 (β-Ga2O3), according to JCPDS
no. 041–1103; except for the peaks labeled α(006) and α(113), which
could be indexed to α-Ga2O3 (JCPDS card no. 006–0503) [49]. The
lower temperature region (in the far downstream) of the horizontal
reactor was crucial in obtaining the mixed-phase (α-β) Ga2O3 films
without deformation to the AGS. The increase in intensity of the
diffraction peaks suggests an improvement in crystalline quality with
increasing deposition temperature. This is because enough thermal en­
ergy was supplied to the adatoms on the substrate and increased the
surface mobility, hence causing the improvement in crystalline quality
[50,51]. Meanwhile, additional diffraction lines could be seen at
elevated temperatures (950 and 1000 ◦ C), featuring an increase in the
polycrystalline nature of the films [50].
The formation of the α-Ga2O3 phase in the lower temperature region
of the reaction chamber is supported by literature. The development of
α-Ga2O3 has been widely reported to be highly favored at temperatures
between 430 and 550 ◦ C [1,24]. Moreover, α-Ga2O3 has recently been
prepared at temperatures between 650 and 800 ◦ C by using various
synthesis technologies [2,52,53]. The formation of the α-Ga2O3 phase
could be linked to the lower substrate temperature and the
oxygen-deficient synthesis atmosphere, as also reported by Lu et al. [2]
Fig. 2. (a) XRD patterns of mixed-phase (α-β) Ga2O3 films prepared on amorphous glass substrates at different temperatures (◦ C), (I) 850, (II) 900, (III) 950, (IV)
1000; (b) FWHM and crystallite sizes of the (111) peak as a function of deposition temperature.
3
Materials Science in Semiconductor Processing 121 (2021) 105361
who obtained Ga2O3 α-β bi-phase films under lower oxygen partial
pressure via pulsed laser deposition method. Interestingly, the growth of
mixed-phase Ga2O3 is rarely reported in the literature by using oxide
powder-source CVD because of the high deposition temperature
required to evaporate the precursor, which does not favor the formation
of the α-Ga2O3 phase [49,53,54].
Crystallite size D was estimated using Scherrer formula, D = 0.9λ/
β cos θ [30,55], while XRD-morphology index (XRD-MI) was evaluated
by the relation MI = βh /(βh + βp ), where β is full width at half maxima
(FWHM), θ is peak position, λ is X-ray wavelength (= 0.15406 nm), βh is
the highest FWHM of the diffraction peak at a particular value of D and
βp is the value of the particular peak for which the MI has to be calcu­
lated [31,56]. D was found to increase as follows, 24.43, 34.26, 36.23,
and 41.76 nm with rising temperature (see Fig. 2(b)), whereas MI was
found to increasingly vary as, 0.369, 0.451, 0.465 and 0.500 with
increasing D and deposition temperature. This demonstrates that MI has
a direct relationship with D and an inverse relationship with specific
surface area [56]. The increasing D could be attributed to improvement
in crystalline quality and led to diffraction line narrowing from 5.923 ×
10− 3 to 3.465 × 10− 3 rad with rising temperature (see Fig. 2(b)) [57,58].
This trend of variation of D with temperature has also been reported
for other materials such as ZnO thin films prepared by radio frequency
magnetron sputtering [59] and sol-gel dip-coating [60], PbSe thin films
produced by chemical bath deposition [61] and Sol-gel prepared cobalt
ferrite nanocomposites [62]. The relationship between increasing D
with elevated temperature could be due to the following reasons: (i) The
increase in the rate of deposition reaction at higher temperatures caused
D to grow faster, resulting in larger size [61]. (ii) Grain coalescence at
higher temperature [60]. (iii) The emergence of the smaller particles
into larger ones, resulting from the potential energy difference between
small and large particles, which occurred through surface diffusion [59].
3.2. Surface morphology
Fig. 3 shows the surface morphology of the Ga2O3 α-β bi-phase
nanomaterials prepared at different temperatures. The films exhibit
facetted aggregates morphology with different growth orientations. The
P.R. Jubu et al.
wool-like patches seen scattered on the solid aggregates are formed due
to Ga-deficiency and excess O. The facetted aggregates are deficient in O
as compared to the wool-like structures. It could be seen that the NSs of
Fig. 3(a and b) prepared at lower temperatures of 850 and 900 ◦ C have
some smaller pieces of nanoaggregates due to unsaturated growth,
which can be ascribed to lower stoichiometry (see inset of Fig. 3(e)).
This is because evaporation of the source powder at lower temperature
was slow and some amount of the source was left in the boat after
growth time had elapsed. The NSs of Fig. 3(c and d) are bigger due to
higher stoichiometry and complete evaporation of the source material at
higher deposition temperatures of 950 and 1000 ◦ C.
Cross-section measurement by FE-SEM showed increasing film
thickness with rising deposition temperature because of the increasing
amount of Ga2O3 material on the surface (see inset Table of Fig. 3(e)).
The gradual increase in the amount of Ga2O3 with elevating temperature
is proposed to be responsible for the increase in XRD peak intensity,
which signifies an improvement of crystalline quality [63] (see Fig. 2
(a)). Composition analysis by EDX showed increasing Ga and decreasing
O atomic percent (at.%) on the produced films with rising deposition
temperature. This led to a decrease of oxygen-metal (O/Ga) atomic ratio
from 1.204 to 1.077 with increasing film thickness. The O/Ga is slightly
below the stoichiometry of 1.50, suggesting the sub-stoichiometric na­
ture of the Ga2O3 films prepared in an oxygen-deficient strong
reducing-ambient growth environment.
The synthesis of the NSs in an oxygen-deficient environment pro­
ceeded by vapor-solid growth mechanism. The transfer of the vaporized
species to the substrate was enabled by the temperature gradient along
the horizontal fabrication line (see Fig. 1). Ga2O3 powder was reduced at
high temperature by H2 gas to release Ga(g) and H2O(g) (Eq. (1)) [64].
The vaporized species moved by temperature gradient, being assisted by
H2 partial pressure to aid deposition on the AGS located in the lower
temperature region of the reaction chamber. The deposited small Ga
droplets then undergo oxidation by H2O(g) plus the residual O2(g) in the
horizontal reactor to form small Ga2O3 nuclei (Eq. (2)) [65]. These small
Ga2O3 nucleation centers provide energetically favored sites for the
adsorption of incoming Ga atoms. The deposition process of the Ga
atoms, which was followed by the oxidation and growth processes was
Fig. 3. Top-view FE-SEM images of mixed-phase Ga2O3 films: (a) 0.723-μm-thick film prepared at 850 ◦ C, (b) 1.058-μm-thick film at 900 ◦ C, (c) 1.107-μm-thick film
at 950 ◦ C, and (d) 1.452-μm-thick film produced at 1000 ◦ C. (e) Representative spectrograph showing elemental peaks, taken from image ‘e’ with the highest Ga at.%.
Inset is the elemental composition of the various films.
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Materials Science in Semiconductor Processing 121 (2021) 105361
continuous until supersaturated Ga2O3 NSs were formed. The NSs grew
in different directions due to the nature of the nucleation sites. The H2
gas used in the experiment played the role of a reducing gas for Ga2O3
powder at high temperature, and also served as a carrier gas.
1000 ◦ C
Ga2 O3 (s) ​ + ​ 3H2 ̅̅→ 2Ga(g) ​ + ​ 3H2 O(g) (1)
< 600 ◦ C
2Ga(g) + O2 (g) + H2 O(g) ̅̅→ Ga2 O3 (s) + H2 (g) (2)
4. Conclusion
In summary, we have investigated the structural and morphological
properties of Ga2O3/glass films prepared by the CVD method using a
Ga2O3 powder source. Films exhibited mixed-phase (α-β) Ga2O3 with
increasing crystallinity and crystallite size due to rising deposition
temperature. Facetted nano-size aggregates morphology of the films and
increasing film thickness was confirmed by microscopy analysis. The O/
Ga ratio was found to increase with decreasing O content in the films as a
result of rising deposition temperature. We believe this research work
will pave the way for the fabrication of Ga2O3 films on amorphous soda
lime glass substrates using the oxide-powder precursor and the high-
temperature CVD technique.
CRediT authorship contribution statement
P.R. Jubu: Conceptualization, Methodology, Investigation, Data
curation, Software, Writing - original draft. F.K. Yam: Conceptualiza­
tion, Methodology, Writing - review & editing, Funding acquisition,
Supervision. O.S. Obaseki: Writing - review & editing, Software.
Yushamdan Yusof: Data curation.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
P.R. Jubu et al. Materials Science in Semiconductor Processing 121 (2021) 105361

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