Recent progress on the electronic

structure, defect, and doping properties of

Ga2O3
Cite as: APL Mater. 8, 020906 (2020); https://doi.org/10.1063/1.5142999
Submitted: 18 December 2019 . Accepted: 28 January 2020 . Published Online: 21 February 2020

Jiaye Zhang, Jueli Shi, Dong-Chen Qi, et al.

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APL Mater. 8, 020906 (2020); https://doi.org/10.1063/1.5142999 8, 020906

© 2020 Author(s).
 APL Materials PERSPECTIVE scitation.org/journal/apm

Recent progress on the electronic structure,

defect, and doping properties of Ga2O3
Cite as: APL Mater. 8, 020906 (2020); doi: 10.1063/1.5142999
Submitted: 18 December 2019 • Accepted: 28 January 2020 •
Published Online: 21 February 2020

Jiaye Zhang,1,2 Jueli Shi,1 Dong-Chen Qi,3 Lang Chen,2,a) and Kelvin H. L. Zhang1,b)

AFFILIATIONS
1
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering,
Xiamen University, Xiamen 361005, China
2
Department of Physics, Southern University of Science and Technology, No. 1088, Xueyuan Blvd., Shenzhen,
Guangdong 518055, China
3
Centre for Materials Science, School of Chemistry and Physics, Queensland University of Technology, Brisbane,
Queensland 4001, Australia

a)
Email: chenlang@sustc.edu.cn
b)
Author to whom correspondence should be addressed: Kelvinzhang@xmu.edu.cn

ABSTRACT
Gallium oxide (Ga2 O3 ) is an emerging wide bandgap semiconductor that has attracted a large amount of interest due to its ultra-large bandgap
of 4.8 eV, a high breakdown field of 8 MV/cm, and high thermal stability. These properties enable Ga2 O3 a promising material for a large
range of applications, such as high power electronic devices and solar-blind ultraviolet (UV) photodetectors. In the past few years, a significant
process has been made for the growth of high-quality bulk crystals and thin films and device optimizations for power electronics and solar
blind UV detection. However, many challenges remain, including the difficulty in p-type doping, a large density of unintentional electron
carriers and defects/impurities, and issues with the device process (contact, dielectrics, and surface passivation), and so on. The purpose of
this article is to provide a timely review on the fundamental understanding of the semiconductor physics and chemistry of Ga2 O3 in terms
of electronic band structures, optical properties, and chemistry of defects and impurity doping. Recent progress and perspectives on epitaxial
thin film growth, chemical and physical properties of defects and impurities, p-type doping, and ternary alloys with In2 O3 and Al2 O3 will be
discussed.
© 2020 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license
(http://creativecommons.org/licenses/by/4.0/). https://doi.org/10.1063/1.5142999., s

I. INTRODUCTION TO Ga2 O3 AND APPLICATIONS
Gallium oxide (Ga2 O3 ) is an emerging ultra-wide bandgap
(UWBG) semiconductor that has attracted a large amount of inter-
est due to its ultra-large bandgap of 4.8 eV, high thermal stability,
and availability of large-scale native substrates for mass production.
Despite the tremendous progress achieved in material development
and devices based on wide bandgap (WBG) semiconductors rep-
resented by SiC and GaN, Ga2 O3 is becoming a competitive can-
didate because of its unique applications such as high power elec-
tronic devices and solar-blind ultraviolet (UV) photodetectors.1 The
most prominent feature of Ga2 O3 is its ultra-large bandgap, which
enables great potential for high electric breakdown field strength (εc )
due to an exponential relationship between the breakdown field and
bandgap value (Eg ), εc = a(Eg )n , (n = 2–2.5).2 Ga2 O3 has a theoreti-
cal breakdown field of up to 8 MV/cm,3 which is attracting attention
from the ultrahigh-power device market (>1 MW) beyond SiC and
GaN based electronics, with specific applications in electrical power
transmission, hybrid propulsion, etc., as shown in Fig. 1.4 Figure 2
shows Baliga’s figure of merit (BFOM) of WBG and UWBG semi-
conductors. Drawn on a log–log specific on-resistance vs breakdown
voltage plot, Baliga’s figure of merit (BFOM) plots the log–log spe-
cific on-resistance vs breakdown voltage and is a type FOM of inter-
est for low-frequency unipolar vertical power switches.5 As shown
in the chart, the BFOM of Ga2 O3 is significantly larger than SiC and
GaN.

APL Mater. 8, 020906 (2020); doi: 10.1063/1.5142999 8, 020906-1

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FIG. 1. Applications of Si, SiC, GaN, and Ga2 O3 for power electronics in terms of
current and voltage requirements.4
Ga2 O3 is also deemed as a rising star in the field of solar-blind
photodetectors, again due to its wide bandgap. The solar-blind ultra-
violet photodetectors have been broadly investigated with the goal of
acquiring precise and accurate information of weak signal by night
and day through the absence of solar-blind region irradiation (200–
280 nm) at the Earth’s surface.6–10 Ga2 O3 based photodetectors pos-
sess the cutoff wavelength range of 250–280 nm, which fulfills the
requirements of detection over a deep ultra-violet (DUV) region and
insensitivity to visible and infra-red wavelength.11,12
From a more practical point of view, the ease of fabrication
of large area native substrates, control of carrier concentration, and
inherent thermal stability also motivate the development of Ga2 O3 -
based devices. N-type doping of Ga2 O3 with Si or Sn has shown good
controllability with a broad range from 1015 cm−3 to 1020 cm−3 .13,14
Although some UWBG semiconductors (such as AlN, c-BN, and
diamond) beat Ga2 O3 in the BFOM chart, their wide utilization is
strongly constrained by practical limits: AlN, c-BN, and diamond
still suffer from a lack of proper substrates for high quality epitaxial
growth.15,16
FIG. 2. Baliga’s figure of merit (BFOM) of common wide bandgap (WBG) and
ultra-wide bandgap (UWBG) semiconductors.3
APL Mater. 8, 020906 (2020); doi: 10.1063/1.5142999
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Although Ga2 O3 based devices have become the focus of
research only in recent years, the explorations of Ga2 O3 may date
back to several decades ago (as shown in Fig. 3). The first report
was on the optical properties of Ga2 O3 in early nineteenth cen-
tury, when the French scientist Lecoq de Boisbaudran found that
“gallium oxide which contains chromium shows a red fluorescence in
a vacuum” right after his discovery of the new element gallium.17
Most of the early publications mainly focused on the basic physi-
cal properties and chemical synthesis of Ga2 O3 .18–22 In 1952, five
different polymorphs of Ga2 O3 , their crystal structure, and phase
stability have been explicitly illustrated by Roy et al.23 The investi-
gations of Ga2 O3 in the period of 1960s–1980s were mostly based
on materials with poor crystallinity or even in amorphous forms,
though some attempts for making Ga2 O3 single crystals started to
appear.24,25 For example, small flasks of single crystals grown by
Chase24 revealed the optical properties of β-phase Ga2 O3 , which
established a bandgap value of 4.7 eV based on the observation of
a band-to-band transition at 270 nm.26 The bandgap values were in
consistency with values measured from bulk crystals and epitaxial
thin films with much better quality.2,27,28 Because a native layer of
Ga2 O3 naturally forms on the surfaces of GaAs and GaN compound
semiconductors, Ga2 O3 thin films, mostly in amorphous or α-phase
polycrystalline forms, were also used as passivating layers for GaAs
based complementary metal-oxide-semiconductor (CMOS) devices
or as anti-reflective coating on GaAs light emitting diodes29–33 and as
dielectric layers on GaN for MOS devices (native Ga2 O3 on the GaN
structure was chemically stable and supposed to be correlated with
the low density of interface states)34 or Ga2 O3 /GaN dielectrics.35,36
Ga2 O3 bulk crystals have also been used as substrates for the growth
of GaN.37–40 Nevertheless, no significant progress has been made in
this attempt because of poor control over the interface, film quality,
and device performance. In fact, it is generally believed that Ga2 O3
plays a negative role in GaAs and GaN technology, in which the
naturally occurred Ga2 O3 must be carefully removed before device
processes.41–43
FIG. 3. Number of publications on Ga2 O3 from 1940 to 2019 (Data: Chemical
Abstracts Service, American Chemical Society).
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 APL Materials
FIG. 4. Photograph of a 4-in. diameter single-crystalline Ga2 O3 wafer.47
From the 1990s to 2010s, significant breakthroughs have been
made in successful growth of a bulk single crystal of high qual-
ity and large size. For example, a large Ga2 O3 single crystal with
size up to 70 mm × 50 mm × 3 mm was realized by the edge-
defined film-fed growth (EFG) method, making EFG one of the
most promising methods for large-scale production.44,45 Commer-
cially available large β-phase Ga2 O3 bulk crystals and wafers with
a size up to 2 in. and 4 in. have been achieved by the Czochral-
ski method46 and EFG method,47,48 respectively. Figure 4 shows
the picture of a 4-in. single crystal grown by the EFG technique.
The availability of large area substrates has in-turn motivated the
homoepitaxial growth of high quality Ga2 O3 thin films with more
sophisticated controlling of doping, defects, modulation doping,
superlattice, etc.13,49–51
Triggered by the growth of large-size bulk crystals, Ga2 O3 -
based device research, including Ga2 O3 based field-effect transis-
tors (FETs),3,48 Schottky barrier diodes (SBDs),4,52–57 and solar-
blind ultraviolet detectors,11,12,58,59 has been experiencing a rapid
rise in the past few years. Some representative device structures
are shown in Fig. 5. In 2012, Higashiwaki et al.60 from the Novel
FIG. 5. Schematic device structures. (a) Schematic cross section of a Ga2 O3 field-plated MOSFET,68 (b) schematic cross section of a Ga2 O3 MESFET,60 and (c) schematic
illustration of a prototype GaN/β-Ga2 O3 p-n junction photodetector.10
APL Mater. 8, 020906 (2020); doi: 10.1063/1.5142999
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Crystal Technology, Inc. reported the metal-semiconductor field-
effect transistors (MESFETs) based on the Ga2 O3 epitaxial layer
grown on the β-Ga2 O3 (010) substrate, which raised a boom in
developing Ga2 O3 -based transistors with a variety of architec-
tures. Ga2 O3 MOSFETs with undoped or n-type channels utiliz-
ing dielectrics such as SiO2 61 or Al2 O3 62 as well as normally off
Ga2 O3 MOSFETs63 have all been extensively investigated.64 Break-
throughs are also achieved in transistor architectures, including
heterostructure field-effect transistors (HFETs),65 current aperture
vertical electron transistors (CAVETs),66 and fin-based vertical junc-
tion field-effect transistors (JFETs).67 Lateral FET with a break-
down voltage of 755 V and channel current of 100 mA/mm has
been demonstrated in 2016.68 It is worth mentioning that two-
dimensional electron gas (2DEG) was achieved in the ternary HFETs
with the modulation-doped β-(Alx Ga1−x )2 O3 /Ga2 O3 interface by
Zhang et al.65
SBDs based on epitaxial layers of β-Ga2 O3 have exhibited
power figure-of-merits (VB 2 /RON ) with great promises, in terms of a
high reverse breakdown field (VB ) together with a low on-resistance
(RON ) value.69 Benefiting from the recent development of homoepi-
taxial growth techniques such as halide vapor phase epitaxy (HVPE)
and low-pressure chemical vapor deposition (LPCVD), capable of
growing thick (>1 μm) and high-quality layers, Ga2 O3 SBDs had
developed rapidly in the last four years.52–55 The breakdown strength
of SBDs based on β-Ga2 O3 has reached up to 4.2 MV/cm with an
extrinsic RON of 3.9 mΩ cm2 ,70 exceeding the theoretical limits of
4H–SiC (2.2 MV/cm) and GaN (3.3 MV/cm).69
Solar-blind UV photodetectors based on Ga2 O3 single crystal
substrates were initially developed by Oshima et al.6 and Suzuki
et al.7 in 2008. Their pioneering works paved the way for the increase
of investigations in this field. Ga2 O3 solar-blind UV photodetectors
have been broadly studied in the types of metal-semiconductor-
metal (MSM) photodetectors, Schottky barrier photodetectors, and
p-n or n-n junction photodiodes using Ga2 O3 bulk crystals,6,7,71,72
films,8,73–76 and micro/nanostructures.9,77 Compared with the widely
used Alx Ga1−x N78,79 and Mgx Zn1−x O,80 whose detectivity is limited
due to their serious alloying composition fluctuation or even phase
segregation, a Ga2 O3 -based photodetector is highly suitable for
practical applications of solar-blind photodetection with improved
photoresponsivity and response speed.12
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 APL Materials
Despite the great progress achieved in multiple technologi-
cal fronts of Ga2 O3 , several challenges still require efforts from
both the academic community and industrial community. There
is still no solid experimental evidence showing the achievement
of p-type doped Ga2 O3 , which makes it impossible to fabricate a
p-n homojunction and, thus, strongly limits its potential in opto-
electronic application. Attempts to make ultra-high breakdown
devices with low turn on voltages still lack valid strategy. Issues
with the device fabrication process including contact, dielectrics,
and surface passivation require further optimization. Although great
improvements have been made in the growth of bulk crystals
and epitaxial layers, more precise control over defects and impu-
rities as well as deeper understanding on the origin of uninten-
tional defects, deep level trap states, carrier transport mechanism,
and so on need more investigations; this is considerably impor-
tant since these defects, doping, and deep level states largely deter-
mine the device operation, output power, threshold voltage, and
carrier mobility by causing carrier compensation, scattering, and
trapping effects.
This review aims to provide an updated account of the semi-
conductor physics of Ga2 O3 in terms of electronic structures, optical
properties, chemistry of defects and dopants, and bandgap engineer-
ing. Recent progress and fundamental understanding on synthesis of
bulk single crystals, epitaxial thin film growth, chemical and physi-
cal properties of defects and impurities, and origin of unintentional
n-type doping, p-type doping, and ternary alloys with In2 O3 and
Al2 O3 were also discussed.
II. SEMICONDUCTOR PHYSICS OF Ga2 O3
A. Polymorphism and crystal structure
There are at least five different polymorphs possible for
Ga2 O3 , including monoclinic phase (β-Ga2 O3 ), rhombohedral
phase (α-Ga2 O3 ), defective spinel phase (γ-Ga2 O3 ), cubic phase
(δ-Ga2 O3 ), and hexagonal phase (ε-Ga2 O3 ). Among these poly-
morphs,
FIG. 6. (a) Rhombohedral crystal structure of corundum-like α-Ga2 O3 with only Oh (blue) coordination Ga. (b) Monoclinic β-Ga2 O3 crystal structure: Ga cations located at
T d (Ga1, green) and Oh (Ga2, blue) coordination. O anions are packed in a distorted cubic structure with two threefold coordinated types (O1 and O2) and one fourfold
coordinated type (O3). (c) Cubic defective spinel lattice structure of γ-phase Ga2 O3 consists of T d (Ga1, green) and Oh (Ga2, blue) coordinated Ga with a ratio of 1:2. (d)
Orthorhombic ε-Ga2 O3 structure.
APL Mater. 8, 020906 (2020); doi: 10.1063/1.5142999
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β-Ga2 O3 is the most stable at ambient environments and, hence, the
most extensively studied phase. The thermodynamic stability of the
five polymorphs was ranked as β < ε < α < δ < γ. For details on
the polymorphs and transition temperature, see, e.g., Ref. 23.
β-Ga2 O3 has a monoclinic crystal structure with a space group
C2/m, as shown in Fig. 6(b). The lattice parameters are a = 12.21 Å,
b = 3.04 Å, c = 5.80 Å, and β = 103.8○ , and the unit cell volume is
208.85 Å3 . A detailed crystal structure of β-Ga2 O3 has been reported
by Åhman et al.81 Briefly, the unit cell of β-Ga2 O3 [Fig. 6(b)]
contains two crystallographically different Ga cations and three O
anions. Half of the Ga cations are in distorted tetrahedral coordi-
nation (Ga1), and the other half are in distorted octahedral coor-
dination (Ga2). O anions are packed in a distorted cubic structure
with two threefold coordinated types (O1 and O2) and one fourfold
coordinated type (O3). Therefore, different bonding environments
could be found in β-Ga2 O3 : the tetrahedrally (T d ) coordinated Ga1
shares bonds with one O1 ion with a bond length of 1.835 Å, one
O3 ion with a bond length of 1.833 Å, and two O2 ions with a
bond length of 1.863 Å. The octahedrally (Oh ) coordinated Ga2
ions share bonds with two O1 ions with a bond length of 1.937 Å,
one O2 ions (1.937 Å), and three O3 ions (one with 2.005 Å and
two within the bc-plane with 2.074 Å). The low crystallographic
symmetry of the monoclinic phase leads to anisotropy of the physi-
cal, optical, and electrical properties, as both predicted theoretically
and observed experimentally. The (010) and (2̄01) planes are the
most commonly used crystal surfaces for device application and thin
film growth.
Polymorphs other than the β-phase are metastable phases and
cannot be grown as bulk crystals from the melt.1 However, they
could be epitaxially grown as thin films stabilized on substrates.
For example, α-Ga2 O3 [Fig. 6(a)] has the same corundum struc-
ture as Al2 O3 , containing only Oh coordinated Ga sites, with lat-
tice parameters of a = 4.98 Å and c = 13.43 Å and a space group
of R3̄c.82 This structure is based on a hexagonally close packed
array of O ions with the Ga cations filling up 2/3 of the cen-
tral Oh sites. High quality epitaxial layers of α-phase Ga2 O3 have
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 APL Materials
been obtained on Al2 O3 (0001) substrates by mist chemical vapor
deposition (mist-CVD),83–85 HVPE,86 and pulsed laser deposition
(PLD).87 Remarkably, FLOSFIA Inc. has succeeded in the growth
of a high-quality α-Ga2 O3 epitaxial thin film on 4-in. Al2 O3 (0001)
substrates by mist-CVD, which makes α-Ga2 O3 a promising phase
for mass production.88
γ-phase Ga2 O3 [Fig. 6(c)] consists of Oh and T d coordinated
Ga with a ratio of 2:1, with a space group of Fd3̄m, and lat-
tice parameters of 8.22 Å.89 It is analogous to the spinel AB2 O4
framework. γ-phase Ga2 O3 thin films have been obtained on
Al2 O3 and MgAl2 O4 substrates by mist-CVD at a growth temper-
ature of 390 ○ C–400 ○ C,90 PLD,91,92 and molecular beam epitaxy
(MBE).93,94
ε-Ga2 O3 is the most elusive Ga2 O3 polymorph. ε-Ga2 O3 was
first reported by Roy et al.23 through heating δ-Ga2 O3 above
500 ○ C, and they assigned it to the hexagonal space group. ε-Ga2 O3
is now accepted as with an orthorhombic structure [Fig. 6(d)]
with lattice parameters of a = 5.0–5.1 Å, b = 8.7–8.8 Å, and
c = 9.2–9.4 Å. Since 2015, single-phase ε-Ga2 O3 thin films have
been obtained on Al2 O3 , AlN, or pseudo-hexagonal substrates by
HVPE,95 MOCVD,96 PLD,97 MBE,98 and mist-CVD.99 Difficulties
in growing phase-pure crystals as well as the disordering nature of
the Ga atoms in the ε phase lead to difficulty in determination of the
structure and properties of ε-Ga2 O3 .
B. Electronic band structure and optical properties
The fundamental electronic structure of β-Ga2 O3 and optical
properties have been studied by numerous first principle calculation
and a few photoemission spectroscopic experiments.100–107 There is
general consensus that β-Ga2 O3 has a direct bandgap of ∼4.87 eV
(though with a slightly smaller indirect bandgap of 4.83 eV). The
conduction band (CB) is mainly composed of delocalized Ga 4s
derived states, giving rise to a dispersive band with a low electron
effective mass, while the valence band (VB) is mainly formed by
occupied O 2p6 derived states with minor hybridization with Ga 3d,
4p, and 4s orbitals.
The band structure of β-Ga2 O3 has been calculated by den-
sity functional theory (DFT),100,101 hybrid HF-DFT,102 and GW
FIG. 7. (a) Band structure of β-Ga2 O3 calculated by Varley et al.107 The conduction band minimum is located at the Γ point, while the valence band maximum is at the M
point. The inset shows the hybridization of Ga 4s orbital and O 2p orbital. (b) Band structure of α-Ga2 O3 calculated by Kobayashi et al.125 The conduction minimum band is
located at the Γ point, while the valence band maximum is at a point between the Γ and S0 points.
APL Mater. 8, 020906 (2020); doi: 10.1063/1.5142999
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methods.103–106 Standard DFT results in an underestimate bandgap
because of the approximations in the calculation of electron
exchange correlation (XC) energy.108–110 Hybrid B3LYP or GW
methods were proven to provide results with better agreement
with the experimental bandgap and lattice parameters. Figure 7(a)
shows the calculated band structure of β-Ga2 O3 by Varley et al.107
using hybrid B3LYP. It can be seen that the bottom of CB, of
mainly the Ga 4s character, shows a highly dispersive feature at the
Γ point.
On the other hand, the top of VB is mainly composed of
localized O 2p orbitals, exhibiting very low dispersion. This results
in a large hole effective mass, in agreement with other calcula-
tions for Ga2 O3 and the situations for other post-transition metal
oxide semiconductors.107 An indirect bandgap of 4.83 eV was found
for Ga2 O3 , with the VB maximum (VBM) located just off the M
point, slightly smaller than the direct bandgap of 4.87 eV at Γ.107
Vertical transitions at the Γ point and VB maximum (VBM) are
both dipole-allowed, but indirect transition probability at VBM are
around one tenth of the strength of direct transition at the Γ point,
as revealed by the dipole matrix analysis. The relatively weak indi-
rect transitions as well as the slight difference between indirect and
direct bandgaps make β-Ga2 O3 a “pseudo-indirect” semiconduc-
tor, as shown experimentally in a sharp absorption edge at roughly
4.9 eV.111
The electronic structure of β-Ga2 O3 was also investigated
experimentally by angle resolved photoemission spectroscopy
(ARPES), showing the VB dispersion along the Γ-A and A-M direc-
tion of the Brillouin zone, as shown in Fig. 8.112 The experimental
VB band structures also exhibit weak dispersion, which fits well
with the calculated band structure. The position of conduction-
band minimum (CBM) was also measured to be at the Γ-point. The
experimental direct and indirect bandgaps are Egdir = 4.9 eV and
Egind = 4.85 eV, respectively.
The VB spectra have been measured by photoemission spec-
troscopy excited with photon energies ranging from 27 eV to 39 eV
by Varley et al.,107,112 80 eV to 130 eV by Lovejoy et al.,113 526 eV
to 556 eV, and 150 eV and 1300 eV by Michling and Schmeißer;114
soft x ray (Al Kα at 1486.6 eV) by Navarro-Quezada et al.115,116
and Swallow et al.;117 and hard x ray (at 8000 eV) by Li et al.118
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FIG. 8. Valence band structure along the A-M (left) and Γ-Z (right) direction of the
Brillouin zone for β-Ga2 O3 measured by angular resolved photoemission spec-
troscopy (ARPES). The experimental bands are shown by black dots. Calculated
band structures based on hybrid DFT calculation are shown as blue lines. The red
marked areas highlight the regions of the direct and indirect gaps.112

Figure 9 shows the comparison of the experimentally measured

VB spectra excited with photon energies of 150 eV and 8000 eV,
with VB density of states (DOS) calculated by DFT. The measured
VB spectra in conjunction with calculated total and partial DOSs
weighted by photoionization cross sections reached the conclusion
that the VB spectra of β-Ga2 O3 mainly consist of O 2p with a band-
width of 7.7 eV. The VB of β-Ga2 O3 shows three main regions:
region I at 0–2 eV below the VBM, region II at 2–6 eV below
the VBM, and region III at 6–8 eV, corresponding to the occu-
pied O 2p6 states slightly hybridized with Ga 3d, 4p, and 4s states,
respectively.
The optical properties of β-Ga2 O3 show notable anisotropy
due to the asymmetry of the crystal structures, as mentioned ear-
lier. This optical anisotropy has come into the view of physi-
cists for a long time. Optical absorption measurement of β-Ga2 O3 FIG. 9. The comparison of VB spectra from the experiment and calculation. (a)
by Tippins in 1965,26 though all conducted with light in the Projected and total density of states (DOS) calculated by DFT. (b) Comparison
of the calculated DOS weighted by photoionization cross sections at 150 eV with
same polarization, still recognized the occurrence of the absorp-
VB spectra measured by 150 eV photon energies. (c) Comparison of the calcu-
tion shoulder which was assigned to different transition energies lated DOS weighted by photoionization cross sections at 8 keV with VB spectra
between T d coordinated Ga1 and O1/O2 [Fig. 10(a)]. A more sys- measured by 8 keV photon energies.118
tematic study on the pleochroism of vapor phase reaction grown
Ga2 O3 single-crystalline platelets was conducted by Matsumoto
et al. using incident light polarized in six different orientations, in transmission spectra. The shoulder transmittances also become
which they observed the highest absorption edge at room temper- stronger with an increase in φ.
ature to be 4.90 eV for E//b shown in Fig. 10(b).119 The absorp- Conditions for material synthesis, defects, and doping also
tion edge in other geometries at room temperature was also mea- show a great influence on optical properties of β-Ga2 O3 . Ueda
sured for E//c and E–b&c with the value of 4.54 eV and 4.56 eV, et al. studied the influence of O2 annealing on Ga2 O3 crystals grown
respectively. Moreover, larger energies were found at 77 K for by the OFZ method and found that the transmittance of Ga2 O3
both E//b and E//c with the corresponding magnitude of 40 meV increased with the elongation of annealing time.120 Galazka et al.46
and 220 meV. reported that Ga2 O3 crystals with lower concentration of free elec-
Optical floating zone (OFZ) grown single crystals were also trons (controlled with different growth atmospheres and dopants by
investigated for pleochroism by Ueda et al.27 Smaller absorption the Czochralski method) showed better transmittance.
edges measured for light polarized E//b and E//c were found to be There are fewer studies on the electronic structure for other
4.90 eV (253 nm) and 4.59 eV (270 nm), as shown in Fig. 10(c). metastable phases of Ga2 O3 , mostly based on theoretical works.
Moreover, increasing the angle φ between E and c could result in A few experimental121,122 and theoretical123–126 results are reported
the appearance of a shoulder at a shorter wavelength in optical for α-Ga2 O3 because it has already been grown by epitaxial

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FIG. 10. (a) Optical absorption spectra of pure β-Ga2 O3 with absorption shoulders measured at room temperature and 77 K.26 (b) Absorption edge of β-Ga2 O3 at room
temperature measured with incident light polarized in six different orientations.119 (c) Optical transmission spectra of β-Ga2 O3 grown by the FZ method measured with light
polarized in different angles.27
methods. The bandgap of α-Ga2 O3 has been measured to be in the
range of 4.9–5.6 eV,83,86,127–129 slightly larger than that of β-Ga2 O3 .
Figure 7(b) shows the calculated band structure of α-Ga2 O3 using
the Heyd-Scuseria-Ernzerh (HSE) hybrid functional reported by
Kobayashi et al.126 The band structure of α-Ga2 O3 is very similar
to that of β-Ga2 O3 , with highly dispersive CBM of Ga 4s. The VB
also exhibits similar flatness as β-Ga2 O3 attributed to localized O
2p. α-Ga2 O3 has the same CBM at Γ as well as VBM at the L or F
point. α-Ga2 O3 is also an indirect semiconductor with a calculated
bandgap of 5.39 eV.
The band structure of ε-Ga2 O3 is also investigated both theo-
retically130–132 and experimentally.132 Similar flatness in VBM and
strong dispersion in CBM are also found in the band structure of
ε-Ga2 O3 as well. The calculated bandgap for ε-Ga2 O3 is reported to
be 4.26 eV by Mulazzi et al.131 using the HSE functional and 4.62 eV
by Pavesi et al.132 using the B3LYP functional. The ARPES results
suggest a lower bandgap value of 4.41 eV,131 while optical absorp-
tion and photoconductivity measurements suggest a bandgap value
of 4.6 eV.132
The band structure of γ-Ga2 O3 was calculated by Gake
et al.133 The calculated direct and indirect bandgaps were 5.30 eV
and 5.15 eV, respectively.
III. MATERIALS SYNTHESIS
High quality bulk crystals and thin films are the starting point
for the fundamental study of the structural, electrical, and optical
properties and for further device fabrication. In the last decade,
achievement in growing large scale and high-quality bulk crystals
has triggered enormous research efforts in the use of Ga2 O3 for
high power electronics and solar-blind photodetectors. Recently,
4-in. high quality β-Ga2 O3 (2̄01) wafers, with the full width at half
maximum (FWHM) for the rocking-curve (4̄02) diffraction below
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17 arcsec and etch pit density (EPD) as low as 103 cm−2 , were
achieved using the EFG-growth method47 and also commercially
available from Novel Crystal Technology, Inc. Furthermore, high-
purity, 1.25 μm-thick (010) β-Ga2 O3 homoepitaxial thin films, with
record-high carrier electronic mobilities of 184 cm2 /V s and low car-
rier concentrations of 2.5 × 1016 cm−3 at room temperature, have
been achieved by MOCVD.134 Using Si, Sn, or Ge as dopants, a con-
trollable n-type doping with free carrier concentration ranging from
1016 to 1020 cm−3 and mobility decreasing from 140 to 40 cm2 /V s
has been achieved for MBE grown homoepitaxial films.13,49 Recently,
using modulation doped β-(Alx Ga1−x )2 O3 /Ga2 O3 heterostructures
to form two-dimensional electron gas (2DEG) at the interface, a
record room-temperature channel mobility of 180 cm2 /V s and
low temperature peak mobility of 2790 cm2 /V s have been demon-
strated.50 Clearly, the availability of large volume and high structural
quality substrates with high electrical and optical parameters at rea-
sonable costs will accelerate the development of devices and circuits,
as in the case of SiC and GaN.
This section will briefly introduce the progress on the growth
technique for bulk single crystals and homo- and hetero-epitaxial
thin films.
A. Bulk single crystals
For the growth of β-Ga2 O3 bulk single crystals, a variety of
techniques have been used, including the Verneuil method, OFZ
method, Czochralski method, Vertical Bridgman (VB) method, and
EFG method.135 Earlier trials of growing Ga2 O3 bulk crystals were
performed by Chase24 and Lorenz et al.25 using the Verneuil method.
The largest dimension achieved by the Verneuil method was 20 × 8
× 2 mm3 with a Hall mobility of about 100 cm2 /V s at room tem-
perature.25 The Verneuil growth of β-Ga2 O3 was merely used in
these days due to the high mechanical stresses caused by the growth
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processes and limited size obtained. The use of the OFZ method
in growing β-Ga2 O3 crystals was initially introduced by Víllora
et al.,136 achieving the growth of substrate-level crystals (∼1 in.) in
2004. The OFZ growth of β-Ga2 O3 has shown great controllability
in both crystal quality and doping level. A wide range of conduc-
tivity (<10−9 S cm−1 to 38 S cm−1 ) could be reached through the
change in growth atmosphere and doping concentration.120 How-
ever, the achievement of a large crystal via the OFZ method is lim-
ited by optical heating.137 The Czochralski growth of β-Ga2 O3 sin-
gle crystals was first reported by Tomm et al.,138 and the growth
of 2-in. in diameter β-Ga2 O3 single crystals was already achieved
by Galazka et al.46 in 2014. However, the growth of larger crys-
tals was impeded by their higher oxygen content during growth.139
Among those methods, EFG is one of the leading candidates to
produce large-size wafers beyond 2-in. with low defect density and
high crystal quality. This method has also been widely used for
mass production of sapphire wafers.140 Recently, Kuramata et al.47
reported EFG-grown β-Ga2 O3 bulk crystals with dimensions of
50 × 55 × 18 mm3 and 110 × 110 × 6 mm3 . The crystals could be
processed into (010), (001), and (2̄01)-oriented 10 × 15 mm2 sub-
strates, as well as (2̄01)-oriented 2- and 4-in. in diameter wafers.
4-in. diameter (001) oriented and 25 × 25 mm2 (010) oriented
single-crystal substrates are currently commercially available from
Novel Crystal Technology, Inc. The substrates can be undoped and
Sn- or Fe-doped with different conductivities. The undoped sub-
strates have carrier concentration below 9 × 1017 cm−3 . The back-
ground n-type carrier concentration can be compensated by addi-
tion of an Fe acceptor to produce semi-insulating substrates; Sn
doping, on the other hand, increases the carrier concentration up to
9 × 1018 cm−3 to make highly conductive substrates. Images of bulk
β-Ga2 O3 crystals grown by OFZ, Czochralski, and EFG methods are
displayed in Fig. 11.
FIG. 11. Bulk β-Ga2 O3 crystals obtained from the following growth methods: (a)
OFZ,136 (b) Czochralski,139 and (c) EFG.47
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B. Epitaxial thin film growth
In order to realize high-performance Ga2 O3 -based devices,
it is essential to grow high-quality Ga2 O3 thin films with con-
trolled density of carriers, defects, and interfaces. From this per-
spective, homoepitaxial growth on available native Ga2 O3 sub-
strates is ideal. The commercial availability of large area Ga2 O3
substrates is one of the advantages of Ga2 O3 in many poten-
tial electrical and optical device applications, compared with
a large mismatch for heteroepitaxial growth of GaN and AlN
on Al2 O3 . Undoped and intentionally doped Ga2 O3 thin films
have been grown by MBE,13,49,51,141–155 MOCVD,134,156–170 mist-
CVD,83,85,121,127,171,172 PLD,111,173–190 HVPE,86,134,170,191–196 and other
techniques such as magnetron sputtering,197–212 atomic layer depo-
sition (ALD),213–217 spin-coating,218–222 and so on. In this section,
we will provide a brief overview of the properties, progress, and
technical challenges of homoepitaxial and heteroepitaxial growth
techniques.
1. MBE
MBE has the potential for generating exceedingly pure and
defect-free films by virtue of the high purity levels available in
commercially available metals and O2 , as well as the low energy
(∼1 eV) of the incident species.223,224 MBE has a typical growth rate
ranging from 12 nm h−1 to 700 nm h−1 and a growth tempera-
ture of 700 ○ C–900 ○ C. The system also houses a reflection high-
energy electron diffraction (RHEED) system, allowing the mon-
itoring of surface structure and morphology in real time during
growth with atomic layer precision.225 MBE is one of the two pre-
dominant growth methods used in GaAs and GaN semiconduc-
tor technology and also the commonly used technique for the epi-
taxial growth of oxide semiconductors, such as In2 O3 226–229 and
Ga2 O3 .13,49,50,230–234
Due to its ultrahigh vacuum (UHV) environment and high
purity source materials, electrically insulating 0.7 μm-thick undoped
films with a smooth surface morphology have been achieved on
(010) Ga2 O3 substrates by MBE.13,49 It has a low residual carrier con-
centration of <2.5 × 1016 cm−3 and carrier mobility of >140 cm2 /V s.
Intentional Sn or Ge doping can induce the n-type electrical conduc-
tivity. For example, by increasing Sn dopant flux, the free electron
concentration can be accurately controlled in a wide range from
∼1016 cm−3 up to 1 × 1020 cm−3 with mobility decreasing from 120
to 40 cm2 /V s.13,49 At present, (010) β-Ga2 O3 homoepitaxial wafers
with a 0.5 μm thick unintentional doping or Si doped Ga2 O3 layer
or 60 nm-thick (Alx Ga1−x )2 O3 (x < 0.23) layer grown by MBE are
commercially available.
Because of the controllability over the growth at atomic pre-
cision, MBE is a promising method to fabricate modulation dop-
ing β-(Alx Ga1−x )2 O3 /β-Ga2 O3 heterojunction or superlattice for an
abrupt band discontinuity and confinement of high mobility two-
dimensional electron carrier at the interface. It has been demon-
strated that β-(Alx Ga1−x )2 O3 solid solution with x as high as 0.20
at 650 ○ C51 and 0.61 at 800 ○ C230,231 or higher can be grown by
MBE. However, the MBE growth temperature is usually limited to
less than 700 ○ C, in order to avoid the decomposition of Ga2 O3
in vacuum.23 Therefore, the Al composition is limited at x = 0.20.
Most interestingly, β-(Alx Ga1−x )2 O3 /β-Ga2 O3 (x = 0.18) modula-
tion doped FETs (MODFETs) have recently been fabricated by
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 APL Materials
MBE50,232–234 and the 2DEG channel mobility has been demon-
strated to be record-high 180 cm2 /V s at room temperature and
2790 cm2 /V s at 50 K, exceeding the highest experimental mobility
values for bulk β-Ga2 O3 .50
2. MOCVD
MOCVD is in essence a CVD system that uses metal-organic
compounds as some of or all its precursors. It is highly scalable with a
large deposition area, suitable for large scale production. At present,
MOCVD is a mature technique for mass production of GaN based
semiconductors and GaN can be epitaxially grown on an 8-in. Si
wafer with reasonably high growth rate.235,236
Recently, benefitting from the low background charge and
compensation concentration by optimizing the growth pressure,
high quality 1.25 μm thick β-Ga2 O3 films with record-high elec-
tron mobility values of 184 cm2 /V s at room temperature and
4984 cm2 /V s at 45 K were achieved on (010) Fe-doped Ga2 O3
substrates using MOCVD.134 The room temperature mobility
approaches the predicted theoretical limit of 220 cm2 /V s.237 Using
Si and Sn as dopants, a controllable carrier concentration ranging
from 1 × 1017 cm−3 to 8 × 1019 cm−3 with a decrease in mobility
from ∼130 cm2 /V s to ∼50 cm2 /V s was achieved.238 The feasibility
of achieving low background impurity concentration and high elec-
tron mobility will inspire more extensive studies on MOCVD for the
fabrication of high-performance power electronics.
Furthermore, due to its higher growth temperature (>800 ○ C)
than that of MBE and smooth surface morphology compared to
that of MBE, MOCVD can grow β-(Alx Ga1−x )2 O3 /β-Ga2 O3 hetero-
junction or superlattice with abrupt heterointerfaces and a higher
Al content (x > 0.4).239 These features in combination with its
high growth rates (0.8 μm/h, much higher than typical 0.2 μm/h
by MBE) make MOCVD very promising for mass production of
β-(Alx Ga1−x )2 O3 /β-Ga2 O3 MODFETs.
Although encouraging results were obtained on (010) sub-
strates, their preparation in large scale remains challenging
because of the limited availability of large size (010) wafers.
Because the (010) substrates must be sliced perpendicularly to
both easy cleavage planes, its largest scale commercially avail-
able from the EFG method (Novel Crystal Technology, Inc.) is
25 × 25 mm2 . Recently, 2 in. diameter cylindrical crystals grown
by the Czochralski method in the [010] direction were demon-
strated.240,241 Thus, potentially 2-in. epi-wafers grown by MOCVD
could be prepared.
3. Mist-CVD
Mist-CVD is a relatively simple and cost-effective technique.
This modified CVD technique uses a fine mist of precursors in a
vapor phase reaction on the substrate.88 It has been extensively used
for the deposition of metal-oxide semiconductors, such as ZnO242,243
and Mgx Zn1−x O.244 Mist-CVD is a promising method to grow
α-Ga2 O3 other than the β-phase on the Al2 O3 substrate.
Due to the similar corundum structure with an in-plane lattice
mismatch of 4.6%, α-Ga2 O3 can be grown on α-Al2 O3 substrates
with a typical edge dislocation density of 7 × 1010 cm−2 but with
a relatively low electron mobility of 2.8 cm2 /V s.83,172,245 By apply-
ing quasi-graded α-(Alx Ga1−x )2 O3 buffer layers, the total density
of dislocations in the α-Ga2 O3 thin films can be further reduced
to ∼108 cm−2 and the electron mobility is increased to 24 cm2 /V s
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with a carrier concentration of 1018 cm−3 .85 Currently, a high qual-
ity 5 μm-thick α-Ga2 O3 layer grown on Al2 O3 (0001) substrates
with a size of 4-in. in diameter is commercially available from
FLOSFIA, Inc.
Furthermore, the solubility of Al in α-(Alx Ga1−x )2 O3 by mist-
CVD (>800 ○ C) is up to x = 0.8.246 Thus, following the successful fab-
rication of modulation-doped β-(Alx Ga1−x )2 O3 /β-Ga2 O3 FETs by
MBE,50 it seems reasonable to realize high performance modulation-
doped α-(Alx Ga1−x )2 O3 /α-Ga2 O3 FETs by mist-CVD. The growth
of highly crystalline α-Ga2 O3 on an inexpensive sapphire substrate
provides an alternative platform to realize high performance power
devices.
On the other hand, taking advantage of the misfit dislocations
and strain accumulated at the interface of the α-Ga2 O3 layer and
Al2 O3 substrate, the epi-structure can be exfoliated from the sub-
strate and mounted on a heat sink.245 This not only simplifies back-
side Ohmic contact deposition but also is important to efficiently
remove the heat from the device. The latter is of particular interest
in the Ga2 O3 technology as this material suffers from poor intrinsic
thermal conductivity.247,248
However, mist-CVD is a relatively new technique (designed
by Kyoto University in 2008)83 and has not been applied to mass-
production of semiconductor epi-wafers. The highest electronic
mobility (24 cm2 /V s) achieved in α-Ga2 O3 is still much lower
than its theoretical value (300 cm2 /V s) and the reported val-
ues of β-Ga2 O3 . In order to utilize α-Ga2 O3 for high perfor-
mance power devices, it is necessary to realize the growth of
high-quality defect-free α-Ga2 O3 thin films, and the realization
requires a steady effort to accumulate technical knowledge of
mist-CVD.
4. PLD
PLD is a versatile technique for the deposition of complex oxide
thin films, heterostructures, and interfaces.223,249 The composition of
targets is preserved in the film, enabling impurity doping or alloying
by varying the composition of targets. However, ions from targets
can be of very high (∼100 eV) energy and, thus, can create point
defects, giving rise to unwanted electrical properties in the epitax-
ial film. Similar to MBE, RHEED can also be used here to monitor
surface structure and morphology.250,251
Recently, a record-high conductivity of 798 S cm−1 with a car-
rier concentration of 1.74 × 1020 cm−3 was achieved by PLD on a
(010) Ga2 O3 substrate from a 1 wt. % SiO2 –Ga2 O3 target.173 Its high
conductivities are critical to address a known problem of Ohmic
contact formation including in β-Ga2 O3 and have extensive impli-
cations on forming low on-resistance for both power switching and
radio frequency (RF) applications. However, the highest mobility
(27 cm2 /V s)173 achieved until now in PLD-grown films is still
much lower than those grown by MOCVD (184 cm2 /V s),134 MBE
(120 cm2 /V s),13,49 and HVPE (149 cm2 /V s) and bulk single crys-
tals grown by EFG-grown (123 cm2 /V s),252 which is likely due to
the ionized impurity scattering of the high density of Si dopants (>3
× 1019 cm−3 ).174 Therefore, steady efforts are required in future to
optimize target compositional control and deposition parameters to
achieve a higher mobility.
Noted that due to high temperature (several thousand degrees)
and high energy of ions and electrons from the target during
growth, the solubility of Al in β-(Alx Ga1−x )2 O3 by PLD is up
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 APL Materials
to x = 0.8 at a relatively low temperature of 400 ○ C,230,253 which
is comparable to x = 0.8 in bulk polycrystals prepared by solid
state synthesis in the 850–1950 ○ C temperature range254 and much
higher than x = 0.18 in thin films prepared by MBE at a typ-
ical temperature of 650 ○ C.51 Therefore, with the characteristics
of the higher solubility of Al at a low growth temperature, it
seems reasonable to push the CB bottom higher by increasing the
Al content in the β-(Alx Ga1−x )2 O3 barrier by PLD, enabling the
enhancement of 2DEG channel mobility and realization of high-
performance modulation-doped β-(Alx Ga1−x )2 O3 /β-Ga2 O3 FETs.
However, the fabrication of such FETs by PLD is still in its infancy,
and much effort is needed to optimize deposition parameters and
conditions.
5. HVPE
HVPE is an old epitaxy growth method that was previously
used for the growth of III-V and GaN compound semiconductors.255
HVPE has the highest growth rate (250 μm/h) for growth of β-Ga2 O3
and is promising for growing thick layers with high productivity.
However, it typically results in rough surface morphology contain-
ing a high density of defects and pits, even when grown on native
substrates.192,195 Therefore, chemical and mechanical polishing pro-
cesses need to be applied prior to device fabrication.248
Recently, 5 μm-thick high quality β-Ga2 O3 layers, with a low
effective donor concentration below 1013 cm−3 , have been homoepi-
taxially grown on (001) β-Ga2 O3 substrates by HVPE with a high
growth rate of 5 μm/h.192 Controllable n-type concentration in the
range of 1015 cm−3 to 1018 cm−3 with the carrier mobility decreas-
ing from 149 to 88 cm2 /V s has been obtained by intentional Si
doping.194 The mobility is almost equal to those of bulk crystals. At
present, (001) β-Ga2 O3 homoepitaxial wafers with a 10 μm-thick Si-
doped layer grown by HVPE are commercially available from Novel
Crystal Technology, Inc.
HVPE can also be utilized to grow high purity α-Ga2 O3 on
Al2 O3 substrates typically at 500–600 ○ C.86 The structural quality of
HVPE-grown α-Ga2 O3 is similar to that of mist-CVD grown films,
with the dislocation density measured by plan-view TEM of typi-
cally ∼1010 cm−2 .75,76 , Using the epitaxial lateral overgrowth (ELO)
technique, the dislocation density in laterally grown wing regions
can also be reduced down to less than 5 × 106 cm−2 .196 The Ge
doped α-Ga2 O3 films show a Hall mobility of 28 cm2 /V s and car-
rier concentration of 3 × 1019 cm−3 ,88 which are comparable to
those of Sn doped films grown by mist-CVD (24 cm2 /V s and
1018 cm−3 ).85
Moreover, as achieved in mist-CVD grown α-Ga2 O3 85 and
III-V compound semiconductors,256,257 inserting a buffer layer can
confine misfit dislocations within the buffer layers and significantly
improve the crystalline quality of the films grown after. Inserting a
buffer layer seems a promising strategy to overcome the lattice mis-
match between α-Ga2 O3 and Al2 O3 and to reduce the dislocations
in HVPE-grown α-Ga2 O3 . The realization of free-standing α-Ga2 O3
wafers by HVPE can also be expected as it happened in GaN industry
and α-Ga2 O3 by mist-CVD.
To summarize this section, as described above, different epi-
taxial techniques have been applied to grow Ga2 O3 thick layers or
thin films. Heteroepitaxial β-Ga2 O3 layers are often polycrystalline,
containing a high density of defects and show low conductivity
<10 S cm−1 and low mobility <1 cm2 /V s.173,188,258,259 Although such
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heteroepitaxial layers might be good enough for some applications,
such as gas sensing218,260 and a solar-blind UV detector,154 high crys-
tal quality layers are still demanded for high-power electronic and
optoelectronic applications.261 Homoepitaxial growth on native sub-
strates is needed to reduce the epitaxial dislocations, defects, and
impurities, and to optimize electrical and optical properties of the
materials. One of the major advantages of the Ga2 O3 technology
is that high quality single-crystal substrates can be grown by melt
methods, as reviewed above. High quality homoepitaxial β-Ga2 O3
layers, with a low residual carrier concentration below 5 × 1016 cm−3
and mobility higher than 150 cm2 /V s, have been grown by MBE,
MOCVD, and HVPE. Their growth kinetics and thermodynam-
ics have been well understood, which are important to achieve
the required structural quality and controllable electrical proper-
ties, with a reasonable growth rate. Among them, MOCVD and
HVPE with a typically high grow rate >0.8 μm/h can be used to
grow thick layers for vertical devices including SBDs, while MBE,
with a control over the growth at atomic precision and a typical
growth rate of 200 nm/h, has promising potential to grow thin films
for lateral devices, such as β-(Alx Ga1−x )2 O3 /β-Ga2 O3 modulation
doped FETs.
The mist-CVD system is relatively new, and its growth kinet-
ics and thermodynamics are not well understood. However, this
growth system and HVPE are both suitable for growth of highly
crystalline α-Ga2 O3 thick films on an inexpensive sapphire. Both
methods can be or are expected to realize free-standing α-Ga2 O3
wafers (>4-in. in diameter) by lift-off technology, providing an alter-
native platform to realize high performance power devices at low
cost and solve the problem of poor thermal conductivity of Ga2 O3
on native substrates, as it happened in GaN industry. However, the
highest reported mobilities for α-Ga2 O3 films grown by mist-CVD
and HVPE are still below 30 cm2 /V s. Thus, much effort is needed to
optimize the growth condition or use a buffer layer at the interface
to reduce the dislocation. Based largely on its relative ease of use and
higher solubility of Al at a low growth temperature, PLD has poten-
tial to enhance the 2DEG channel mobility in modulation-doped
β-(Alx Ga1−x )2 O3 /β-Ga2 O3 FETs.
IV. DEFECT AND DOPING (ELECTRONIC STRUCTURE,
OPTICAL, MOBILITY, AND TRANSPORT)
In the undoped stoichiometric state, Ga2 O3 should be a trans-
parent insulator because of its ultra-large bandgap of 4.87 eV.
However, Ga2 O3 exhibits an unintentionally n-type conductiv-
ity,47,262,263 and the origin of the unintentional doping is still under
debate. Defects such as oxygen vacancies (VO ), hydrogen intersti-
tials (Hi) and substitutions (HO), Ga interstitials (Gai), and other
impurities have been proposed.264–267 Ga2 O3 is also amenable to
n-type doping with Si,268 Sn,47 Ge,13 Nb,269 Ta,270 and so on.
The free electron concentration could be controlled by growth
conditions, post-growth treatment, or intentional doping, in the
range of 1016 –1019 cm−3 for bulk crystals49,268 and in the range of
1014 –1020 cm−3 for epitaxial thin films188,194,258 with a correspond-
ing Hall mobility of up to about 140 and 184 cm2 /V s,13,134,194
respectively. On the other hand, as discussed earlier, p-type dop-
ing in Ga2 O3 would be fundamentally difficult because of the very
flat VBM of O 2p in nature and self-compensation.271–273 Under-
standing the physical properties of defects and impurities in Ga2 O3
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 APL Materials
and in turn controlling them are crucial for increasing device
performance since defects and impurities affect material proper-
ties critical to device operation, output power, breakdown volt-
age, carrier mobility by scattering and trapping effects, lumines-
cence274,275 and charge-trapping,276,277 and a prerequisite for p-type
doping. For instance, Neal et al.278 have carried out a critical assess-
ment of the specific on-resistance (Ronsp ) and breakdown voltage
of Schottky diodes containing defect states at 110 meV below the
CBM, as shown in Fig. 12; to achieve 20 kV breakdown voltage
in Ga2 O3 (comparable to SiC devices), the concentration of these
defects must be below 5 × 1014 cm−3 , while at present, only a
1.1 kV device has been demonstrated with a defect concentration of
1 × 1016 cm−3 .
In this section, we will review the defects and doping chem-
istry in Ga2 O3 and its impact on electrical conductivity, mobility,
and optical properties. We will begin with a brief introduction on
the fundamental semiconductor physics for doping and defects in
oxide materials.
A. Fundamental semiconductor physics of doping
and defects in Ga2 O3
The fundamentals of doping and defects can be understood by
the physics of semiconductors. The electrical conductivity (σ) of a
semiconductor is directly related to its carrier concentration (n) and
carrier mobility (μ), according to the relation σ = neμ, where e is the
elementary charge. These parameters are fundamentally related to
the electronic structure of oxides. n is determined by the intrinsic
ease of generation of mobile carriers (electrons for n-type and holes
for p-type) by defects or dopants. The carrier mobility μ is directly
proportional to the free carrier scattering time, τ, and is inversely
proportional to the carrier effective mass, m∗ , via μ = eτ/m∗ . τ largely
depends on extrinsic factors such as ionized dopants, defects, and
grain boundaries determined by film preparation procedures. m∗ is
an intrinsic property of the materials, a tensor whose components
are obtained from the electronic band structure by analyzing the
FIG. 12. Normalized breakdown voltage (left axis) vs doping concentration for
single-sided junction power devices. The ideal relationship assuming the full-
depletion approximation and 1D electrostatics is shown by the black line. The right
axis indicates the projected absolute breakdown voltage for Ga2 O3 devices for
comparison. Square symbols indicate experimental measurements of devices with
breakdown voltages among the highest reported for each material: Si, SiC, GaN,
and Ga2 O3 .452
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variation of energy (E) with momentum (k). Thus, a highly dis-
persive VBM or CBM gives rise to small m∗ and hence potentially
a high μ.
1. Effective mass and doping
For Ga2 O3 , the top of VB is primarily formed by fully filled
O 2p6 states and the CBM mainly by the unoccupied Ga 4s0
orbitals. The Ga 4s0 derived CBM is the key for achieving a high
n-type conductivity and mobility in Ga2 O3 for the following two
reasons.
First of all, the 4s orbital normally has large spatial distribu-
tions and their wavefunctions overlap with each other [inset in
Fig. 7(a)], leading to a facile pathway for the conduction of elec-
trons. In the view of band structure [Fig. 7(a)], the s orbitals form
a highly dispersive CBM at the Γ point, giving rise to a small m∗ .
m∗ for β-Ga2 O3 have been theoretically predicted to be 0.227–0.242
me (me is the rest mass of an electron),279 0.342 me ,123 0.26–0.27
me ,124 0.28 me ,280 0.27–0.28 me ,106 and 0.22–0.3 me 281 depending
on the calculation methods. Experimental results revealed the m∗
values of 0.28 me ,112,280 0.283–0.288 me for the (010) surface, and
0.276–0.311 me for the (2̄01) surface.282 A small m∗ is also true for
other wide bandgap oxide semiconductors, including In2 O3 ,283–285
ZnO,286,287 and SnO2 ,288,289 which typically have small electron effec-
tive masses of 0.20–0.35 me . On the other hand, the effective masses
for holes are as large as 10 me , suggesting the fundamental limita-
tion to obtaining highly mobile holes at the VBM. This is reflected
in part by numerous attempts at p-type doping of ZnO290–292 and
In2 O3 ,293,294 but no encouraging results have been achieved so
far, and there are still problems concerning the reproducibility of
the results.
Second, owing to the Ga 3d contraction, the energy of Ga 4s
is relatively lower than those of pre-transition metals (e.g., MgO).
This gives rise to a relatively high electron affinity that facilitates
n-type doping.295 Ga2 O3 has an electron affinity of 4.0 eV,296 com-
pared to 1.4 eV for MgO.297 For Ga2 O3 , substitution of Ga3+ by
Si4+ , Ge4+ , and Sn4+ introduces dopant energy levels with ionization
energy less than ∼50 meV below the CBM.298 The extra electrons can
be easily activated into the CBM as free carriers, inducing a signifi-
cant increase in conductivity. The activation energy (Ea ) for donors
depend on the doping concentration (N d ), i.e., Ea decreases with an
increase in N d , resulting from a combined effect of screening of the
dopant’s Coulomb potential by free carriers and charged impurities
and of spatial fluctuations of the CB edge induced by the potentials of
randomly distributed charged impurities. Generally, ΔEa decreases
according to
ΔEa = ΔE0 − βNd 1/3 ,
where ΔE0 is the activation energy for isolated donors and β
is a constant. For example, Irmscher et al.299 measured Ea for
Si doped Ga2 O3 bulk crystals grown by the Czochralski method
with N d from 1.25 × 1017 cm−3 to 9 × 1017 cm−3 ; Ea decreases
from 25 meV to 16 meV, as shown in Fig. 13. The extrapo-
lation of this dependence to zero concentration Nd yielded for
the ionization energy Ea of isolated donors a value of about
36.3 meV.
With more doping, the Fermi level (Ef ) moves up into the CB
and the materials ultimately become a degenerate semiconductor
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FIG. 13. Measured donor ionization energies (E a ) vs the cubic root of the donor
concentrations (Nd ). The extrapolation of this dependence to zero concentration
yielding the ionization energy Ea for isolated donors of about 36.3 meV.299
with metallic transport behavior [Fig. 14(a)]. The critical carrier con-
centration nc for the transition from an insulating state to metallic
state is defined by the Mott criterion, (nc )1/3a0 ∗ > 0.26, where a0 ∗
is the Bohr radius. Taking Sn doped Ga2 O3 , for example, the lit-
erature suggests that the static dielectric constant is ε(0) = 10.2300
and an electron effective mass is m∗ = 0.28 me ,112,280 giving an
effective Bohr radius of a0 ∗ = a0 ε(0)/(m∗ /me ) = 1.92 nm. Thus, nc
is calculated to be 2.48 × 1018 cm−3 . For example, a carrier con-
centration of 1.74 × 1020 cm−3 can be achieved, together with a
typically electron mobility of 26.5 cm2 /V s, yielding a high con-
ductivity of 732 S cm−1 .173 It should be noted that dopants and
other defects such as vacancies or interstitials in the lattice behave as
point scatters of electrons and such scattering events limits electron
mobility.
The free electrons in the CB can oscillate with an external
electromagnetic field, such as the free electrons in metals (plasma
FIG. 14. (a) Schematic electronic structure of Ga2 O3 (left), showing the Ga 4s derived CB and O 2p derived VB, and degenerately Sn doped Ga2 O3 (right), which displaces
the Fermi level (Ef ) above CB minimum, making the system metallic; the filling CB increases the optical bandgap by a Burstein–Moss shift. (b) Transmittance spectra of
β-Ga2 O3 single crystals obtained by the Czochralski method with various free electron concentrations. The absorption in the NIR region is negligible when free electron
concentration is less than 3.5 × 1017 cm−3 . While larger than 2.2 × 1018 cm−3 , the absorption at NIR is strong.46
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oscillations). Below the plasma energy, any material exhibits a high
reflectivity. The plasma frequency, ωp , is given by
ne2
ω2p = ,
m∗ ε(∞)ε0
where n is the free carrier density, m∗ is the electron effective
mass, and ε0 is the permittivity of free space. The plasma frequency
depends on the carrier concentration.301,302 For a carrier concentra-
tion of order 1018 cm−3 , the plasma energy is typically in the near-
infrared (NIR) region at around 0.4–0.7 eV. Bluish coloration due
to reflectivity in the NIR has typically been observed for electrically
conductive specimens.46 Insulating specimens were colorless and,
therefore, transparent in the UV, visible, and IR regions, as shown in
Fig. 14(b). Therefore, the “optical window” for doped Ga2 O3 is set at
short wavelengths by its optical bandgap and at longer wavelengths
̵ p ).
by its reflectivity plasma edge (hω
2. Intrinsic mobility limits in Ga2 O3
We now turn back to discuss the electron mobility in Ga2 O3 .
As mentioned above, β-Ga2 O3 has a small m∗ of 0.28–0.33 me
because the CBM derives mostly from the dispersive Ga 4s states.
The m∗ of β-Ga2 O3 and its character are quite similar to those
of GaN.303 One may initially expect that the electron mobility of
Ga2 O3 is similar to that of GaN of 1500 cm2 /V s.237 However, so far,
the best room temperature mobility in β-Ga2 O3 is in the range of
150–184 cm2 /V s,134,194 nearly an order of magnitude lower
than GaN. One critical question is whether the reported lower
mobilities in β-Ga2 O3 are intrinsic or extrinsic which can be
improved by eliminating defects/impurities. Ma et al.237 performed
experimental and theoretical analyses on temperature dependent
transport properties of Ga2 O3 . They found a strong electron–
phonon interaction in Ga2 O3 because of the high ionic Ga–O
bonds. For pure β-Ga2 O3 with low density of defects and
impurities (<1017 cm−3 ), the electron mobility in β-Ga2 O3 is
limited by the polar optical phonon (POP) scattering with a
maximum of 220 cm2 /V s at room temperature; for doped
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β-Ga2 O3 with a higher density of defects and impurities, the electron
mobility is limited by scattering at ionized impurities. POP scatter-
ing was also reported by Ghosh and Singisetti304 and Parisini and
Fornari.305
3. Deep level states
Several deep level states in β-Ga2 O3 bulk crystals and thin
films have been identified using deep level transient spectroscopy
(DLTS), deep level optical spectroscopy (DLOS), and combination
with other techniques and DFT calculations. Using DLTS, Irmscher
et al.299 found three deep trap states in undoped β-Ga2 O3 crystals
grown by the Czochralski method, including E1 with energy level
located at 0.54 eV below CB (EC -0.54 eV), E2 at 0.72 eV below CB
(EC -0.72 eV), and E3 at 1.04 eV below CB (EC -1.04 eV). E2 is the
dominating trap with a concentration of 2–4 × 1016 cm−3 and is
detected in all samples. E3 is only present in some samples pre-
pared with specific conditions but with comparable concentration
to E2 . E1 has a concentration of one order of magnitude lower than
that of E2 and E3 (3 × 1014 –6 × 1015 cm−3 ). The deep level states
can act as compensating acceptors. Although more works should be
done to identify the microscopic and chemical nature of the deep
level states, Irmscher et al.299 proposed that transition metal impu-
rities such as Fe3+ and Co2+ may be responsible for some of the
deep traps because EPR detected the presence of Fe3+ and Co2+ in
their samples.
Zhang et al.306 performed DLTS and DLOS to probe the deep
level states in bulk β-Ga2 O3 single crystals grown by EFG, in which
five distinct deep states have been detected. Their energy levels and
concentrations are shown in Fig. 15. Three states, E1 (EC -0.62 eV), E2
(EC -0.82 eV), and E3 (EC -1.00 eV), detected by DLTS are very simi-
lar to those found in the work by Irmscher et al.299 Moreover, DLOS
allowed to identify another two deeper states than DLTS, including
E4 (EC -2.16 eV) and E5 (EC -4.4 eV, i.e., 0.43 eV above VB). E2 and
E5 are the dominant ones, with a concentration of ∼1016 cm−3 . The
authors also speculated that E2 may be associated with either SnGa
or VO point defects, and E4 may be with Ga vacancies (VGa ). How-
ever, more work is needed to verify these interesting but speculative
assignments.
Ingebrigtsen et al.307 combined DLTS, proton radiation, sec-
ondary ion mass spectrometry (SIMS), and hybrid DFT calculations
FIG. 15. Summary of the distribution of deep level defect states detected by both
DLTS and DLOS in the same EFG-grown β-Ga2 O3 (010) materials.453
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to study the deep level states in β-Ga2 O3 synthesized by differ-
ent methods, including EFG single crystals and homoepitaxial film
grown by MBE and HVPE. For the EFG single crystals, they found
similar trap distribution to those measured by Irmscher et al.299
and Zhang et al.306 with E2 dominating. However, for the epitaxial
films by MBE and HVPE, E2 has 2 orders of magnitude lower con-
centration. As further confirmed by SIMS measurements, they con-
cluded that E2 has an extrinsic origin, associated with residual Fe3+
impurities occupying Ga sites. More interestingly, their results also
revealed another deep state, E2 ∗ at 0.72 eV below CB (EC -0.72 eV).
E2 ∗ was identified as having an intrinsic origin, perhaps from Ga
vacancies or its complexes. Similar results were also reported by
Polyakov et al.308 based on HVPE-grown β-Ga2 O3 epitaxial films
which exhibit E1 , E2 , and E3 deep states near EC -0.6 eV, EC -0.75 eV,
and EC -1.05 eV, but the concentration of these traps in the HVPE
film is 1–2 orders of magnitude lower than that in bulk crystals.
However, proton irradiation increases the concentrations of E2 and
E4 states, suggesting that these states are associated with intrin-
sic defects, different from the conclusion by Irmscher et al.299 and
Ingebrigtsen et al.307
To summarize this part, although several deep level states in
bulk crystals and thin films of β-Ga2 O3 have been identified, their
physical origin remains elusive. More works such as high-resolution
photoemission spectroscopy, photoluminescence, and DFT calcula-
tions should be performed to clarify their origins. Knowledge of the
natures of these types of deep levels is critical for further developing
Ga2 O3 -based optoelectronic devices.
B. Unintentional doping and intrinsic defects
(oxygen Vo and hydrogen Hi and Ho )
It is often observed that β-Ga2 O3 bulk crystals and thin films
exhibit an intrinsic n-type conductivity (with a background free
electron concentration), despite the absence of intentional dop-
ing.47,262,263 Such unintentional n-type conductivity is also com-
monly observed for other wide bandgap oxide semiconductors
(ZnO,273,309 In2 O3 ,226,283,310 and SnO2 311,312 ). Table I summarizes
unintentional doping electron concentration and mobility for
Ga2 O3 single crystals (bulk and epitaxial thin films) grown by differ-
ent methods and at different conditions. The resulting electron con-
centrations between 1016 cm−3 and 1019 cm−3 would correspond to
a donor concentration of 0.000 01%–0.01%. Despite intense research
in the last few years, the origin of the unintentional doping is still
not settled. The proposed electron donors include oxygen vacancies
(Vo ), hydrogen, Ga interstitial (Gai ), and other impurities from the
material synthesis process, but no conclusive agreement has been
reached yet.
1. Oxygen vacancies (Vo )
It is often experimentally observed that the growth of Ga2 O3
or post-growth annealing in high oxidizing environments reduces
the free electron density whereas in reducing conditions (nitro-
gen, hydrogen, or ultra-high vacuum) leads to an increase in
n-type conductivity. Table I summarizes the basic electrical prop-
erties of β-Ga2 O3 bulk crystals grown by different methods in dif-
ferent environments. For example, as further shown in Fig. 16(a),
Ueda et al.262 synthesized β-Ga2 O3 bulk crystals by the floating zone
method and showed that the conductivity strongly depends on the
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TABLE I. A summary for unintentional doping electron concentration and mobility for basic electrical properties of β-Ga2 O3 single crystals (bulk and epitaxial thin films) grown
by different methods and at different conditions.

Sample Growth Growth Electron Electron mobility Conductivity

type Substrate method (T/○ C) O2 pressure/flow conc. (cm−3 ) (cm2 /V s) (S cm−1 ) References

Bulk ... Verneuil ... ... 1018 80 30 315

Bulk ... OFZ ... 0.12 m3 h−1 5 × 1018 ... 38 262
Bulk ... OFZ ... 6 × 10−3 m3 h−1 1.4 ± 0.5 × 1017 60 ± 20 12 446
Bulk ... OFZ ... 2 × 105 Pa 5 × 1017 88 7 263
Bulk ... OFZ ... ... 7.7 × 1016 172 2 447
Bulk ... EFG ... 2 × 104 Pa 2 × 1017 ... ... 47
Bulk ... EFG ... 0 3.9 × 1016 107 0.67 135
Bulk ... CZ ... 0 5.2 × 1017 126 10.5 448
Bulk ... CZ ... 2 × 104 Pa 3.5 × 1017 121 6.7 448
Bulk ... CZ ... 6 × 102 Pa 1 × 1018 86 14 46
Bulk ... CZ ... 8 × 102 Pa 0.4–4.8 × 1017 100–144 0.9–8 46
Bulk ... CZ ... 1.2 × 103 Pa 0.98–22 × 1017 80–152 5–11 46
Bulk ... CZ ... 4.4 × 103 Pa 2.8–6 × 1017 114–127 17–100 46
Bulk ... CZ ... 0.8–3.5 × 105 Pa 0.5–6 × 1017 80–90 2–6 240
Thin films Ga2 O3 (010) MBE 600 <2.5 × 1016 >140 ... 49

O2 flow in the growth atmosphere: the conductivity is lower than
10−9 S/cm when grown in pure O2 atmosphere, increases with a
decrease in the O2 content, and reaches a large conductivity of
38 S/cm with n = 5 × 1018 cm−3 at an N2 /O2 ratio of 0.4/0.6.
On the other hand, the conductive crystals became insulating after
annealing in O2 . Furthermore, the dependence of conductivity on
oxygen partial pressure (PO2 ) was investigated by Cojocaru and
Alecu313 and Fleischer and Meixner314 using Ga2 O3 polycrystalline
thin films: Ga2 O3 shows a characteristic (PO2 )−1/4 dependence of
conductivity with a relation of σ ∼ (PO2 )−1/4 . Because of the inverse
correlation between conductivity and oxygen partial pressure, the
n-type conductivity in Ga2 O3 was commonly attributed to the
presence of Vo.262,264,275,315,316
In order to preserve the charge neutrality, a Vo captures two
electrons and is denoted as a neutral vacancy Vox . Free carriers can
be generated, by single or double ionization of Vox , resulting in Vo●
or Vo●● , respectively. The donor state energy levels were experimen-
tally determined to be located only ∼0.02–0.03 eV below the CBM.315
Aubay and Gourier317 synthesized β-Ga2 O3 single crystals using the
Verneuil method. The samples showed a very high conductivity of
200 S/cm and slightly blue color, when synthesized under reduc-
ing conditions (H2 /O2 flow rate of 2:3). In normal conditions, the
sample was insulating with a conductivity of 10−6 S cm−1 and trans-
parent. They also performed a detailed EPR study on the magnetic
bistability and Overhauser shift of conduction electrons and con-
cluded that Vo forms a partially occupied shallow impurity donor
and is responsible for the low-temperature conductivity. Using EPR,
Yamaga et al.264 provided further microscopic evidence that among
the three oxygen sites, the one in fourfold coordination acts as a shal-
low donor, trapping a single unpaired electron (Vo● ), i.e., each Vo
donates one delocalized electron responsible for conductivity, while
the other is localized.

FIG. 16. (a) The electrical conductivity of the β-Ga2 O3 sin-

gle crystals along the b axis as a function of the O2 flow
rate. The total gas flow rate (N2 +O2 ) was 0.2 m3 h−1 . The
closed circles and the open square refer to samples grown
from undoped and Sn-doped Ga2 O3 rods, respectively.120
(b) Hall free carrier concentration vs the dopant concen-
tration of Si and Sn doped β-Ga2 O3 single crystalline epi-
taxial layers obtained by secondary-ion mass spectrometry
(SIMS).454

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However, this assumption was questioned by Varley et al.298
and others318 who performed first-principle calculations based on
hybrid DFT of various impurities and Vo in β-Ga2 O3 . Accord-
ing to these calculations, Vo acts as a deep donor with an ioniza-
tion energy of more than 1 eV and, thus, cannot be the source
of n-type conductivity. This would be similar to the case of other
oxide semiconductors (In2 O3 ,319 SnO2 ,311,312 and ZnO273,309 ), where
the energy level of Vo is too deep to be ionized for n-type
conductivity.320 The deep level states of Vo in Ga2 O3 may also
be associated with the observations of blue luminescence emis-
sions arising from the recombination of a localized donor state
(attributed to Vo) with trapped hole states,274,321 a high concen-
tration trap state at 0.82 eV (likely related to the deep level state,
e.g., Vo) below the CBM of Ga2 O3 detected by DLTS,306 and depth-
resolved cathodoluminescence spectroscopy and surface photovolt-
age spectroscopy.322
2. Hydrogen interstitials (Hi ) and substitution (HO )
Alternatively, hydrogen impurities were proposed to act as
shallow donors in Ga2 O3 and can be present both as an intersti-
tial species (Hi ) and as a substitutional donor at the oxygen vacancy
site (HO ).298,323 Hi has low formation energy under both O-rich
and O-poor conditions, indicating that it will easily be incorpo-
rated as an unintentional impurity, when hydrogen is present in
the growth or annealing environment. However, HO has a low
formation energy only under O-poor conditions. There is also
experimental evidence that hydrogen may be a shallow donor in
Ga2 O3 ,324 based on its implanted muonium counterpart whose
properties mimic those of hydrogen form shallow donors and EPR
of single-crystal samples. Hydrogen impurities are suggested as shal-
low donors, in general, in many wide bandgap oxide semicon-
ductors such as ZnO,325 In2 O3 ,326 and SnO2 .327 It was theoreti-
cally predicted that Hi and HO were shallow donors in In2 O3 and
further proved by King et al.328 based on muon-spin-resonance
experiments.
However, the hydrogen shallow donor model has been ques-
tioned by Polyakov et al.329 based on hydrogen plasma treatment
of β-Ga2 O3 , after which they observed a pronounced decrease
in the concentration of shallow donors that provide free elec-
trons, which did not corroborate the theoretical prediction that
hydrogen in β-Ga2 O3 should be an efficient shallow donor. There
is a possibility that hydrogen forms electrically active complexes
with deep native defects, such as VGa , and gives rise to donor
compensation.
3. Ga interstitials (Gai )
Gai are shallow donors and could act as an alternative source
of n-type conductivity, but the recent calculation suggests that Gai
is highly mobile and it has a large formation energy (>2.5 eV)
at extreme oxygen-poor growth conditions, which make them less
likely to be present.266,318
4. Other impurities
In addition to VO , hydrogen, and Gai , residual impurities (Si,
C, F, etc.) are present in bulk crystals, typically at a concentration
of a few ppm by weight.47 The sources of the residual impurities
may come from starting precursors used for synthesis (all growth
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methods), containers and crucibles for growth, flux composition
(solution methods), and thermal insulation and furnaces (all growth
methods). Some of the residual impurities could be electrically
active, e.g., Si, F, and others not, but they may affect the electri-
cal properties (e.g., mobility) indirectly through structural qual-
ity. For example, it has been shown that Si is the main impurity
present in high-purity Ga2 O3 powders330 and single crystals.275
The Si impurity concentrations are determined at 10–20 ppm
(weight) for 4N (99.99%) purity Ga2 O3 and 0.05–1.8 ppm for
6N (99.9999%), which corresponds to a Si concentration of
1–3 × 1018 cm−3 and 1016 –1017 cm−3 . These values would give
comparable electron density observed in unintentional doped
Ga2 O3 .
C. Intentional n -type doping
Controllable n-type conductivity can be realized by intentional
doping with group IV elements (e.g., Si, Ge, and Sn)13,47,268 and tran-
sition metals (e.g., Nb, Zr, and Ta)269,270 as shallow donors, or by
Mg and Fe compensating the n-type conductivity. Si and Sn are
the most extensively studied dopants because of their low activation
energy (7.4–60 meV for Sn,331,332 16–50 meV for Si,237,278,299,305,333
and 17.5–30 meV for Ge334,335 ) and compatibility with epitaxial
growth processes. Using Si, Sn, and Ge as dopants, a wide range
of free carrier concentration (n) from 1016 up to 1019 cm−3 and a
peak mobility of 152 cm2 /V s have been achieved for bulk crys-
tals, and n from 1015 cm−3 to 1020 cm−3 and a peak mobility of
184 cm2 /V s have been achieved for epitaxial thin films. Table II pro-
vides an overview for the basic electrical properties (conductivity,
carrier concentration, and mobility) of doped Ga2 O3 bulk crystals
and epitaxial thin films grown by different methods and dopants.
Varley et al.298 have performed hybrid DFT calculations and showed
that Si, Sn, and Ge form shallow donor states close to the bot-
tom of the CB of Ga2 O3 ; all three dopants have lower formation
energy under oxygen-poor conditions, whereas secondary phases
of SiO2 , GeO2 , and SnO2 preferentially form under oxygen rich
conditions.
Si and Ge preferentially substitute the T d coordinated Ga1
site, while Sn prefers the Oh coordinated Ga2 site because of
its large cation size. Sn at Ga2 sites has been confirmed by
x-ray absorption spectroscopy (XAS).336 However, scanning tun-
neling microscopy/spectroscopy (STM/STS) on Si-doped EFG sin-
gle crystals suggested an even distribution of Si between the Ga1
and Ga2 sites.337 Si at different coordination may have differ-
ent activation energies. Some authors suggest that Si at Ga2 sites
may not be electrically active268 or with an activation energy
of 120 meV.134
Figure 16(b) shows the total doped concentration determined
by SIMS and carrier density determined by Hall effect measure-
ments in van der Pauw geometry at room temperature.238 It showed
that free electron density systematically increases with dopants
for dopants <1019 cm−3 , indicating that most of the dopants are
activated to give free carriers. At higher dopant concentration,
the actual carrier concentration is limited by the solubility of the
dopants, either through the formation of secondary phases of oxides
(e.g., SiO2 and GeO2 ) or through low incorporation of Sn due to
their high vapor pressure. On the other hand, it should be noted
that the carrier concentration is also strongly influenced by other
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TABLE II. A summary for the basic electrical properties of doped β-Ga2 O3 single crystals (bulk and epitaxial thin films) grown by different methods and at different conditions.

Sample Growth Electron Electron mobility Conductivity

type Substrate method Dopant conc. (cm−3 ) (cm2 V−1 s−1 ) (S cm− 1 ) Reference

Bulk ... OFZ 10−5 –10−1 mol. % Si 5 × 1016 –5 × 1018 ∼100 0.9–40 449
Bulk ... OFZ 2 mol. % SnO2 2.26 × 1017 65 23 263
Bulk ... OFZ 5 mol. % SnO2 7.12 × 1017 49 56 263
Bulk ... OFZ SnO2 1 × 1018 80 13 340
Bulk ... OFZ Mg ... ... 1.7 × 10−12 447
Bulk ... EFG SiO2 4.9 × 1018 93 7.1 450
Bulk ... EFG SiO2 1 × 1019 ... ... 47
Bulk ... CZ 800 wt ppm Sn4+ 3–10 × 1018 35–52 17–100 46
Bulk ... CZ 6–28 wt ppm Mg2+ ... ... ... 46
Bulk ... Bridgman 150–400 wt ppm Sn4+ 5–10 × 1018 30–40 ... 240
Thin films Ga2 O3 (010) MBE Ge 5 × 1016 –1020 120–40 ∼0.952–635 13
Thin films Ga2 O3 (010) MBE Sn 1016 –7.5 × 1019 97–39 ∼0.154–464.3 13
Thin films Ga2 O3 (010) MBE Sn 1016 –1019 140–33 ∼0.22–532.8 49
Thin films Ga2 O3 (010) MOCVD Si 1017 –8 × 1019 130–50 ∼2.06–634 238
Thin films Ga2 O3 (010) MOCVD Si 2.5 × 1016 184 ∼0.73 344
Thin films Ga2 O3 (010) PLD 0.025–1 wt. % SiO2 3.25 × 1019 –1.75 × 1020 20–30 ∼732 345
Thin films Ga2 O3 (001) HVPE Si 1015 –1018 149–88 ∼0.076–16.67 194
Thin films Ga2 O3 (010) HVPE Si 3 × 1016 –1020 124–50 ∼4.76 × 10−3 –800 347

defects promoted by different conditions. For example, VGa or oxy-
gen interstitials (Oi ) formed under metal-poor/oxygen-rich condi-
tions may act as “electron-killers,” counteracting T d doping; like-
wise, under oxygen-poor/metal-rich conditions, hydrogen, Gai , or
VO may provide extra free electrons, although their roles are still
controversial as mentioned above.
The electron mobility shows an inverse correlation with the
free electron concentration. This is valid for both bulk crys-
tals25,27,46,139,335,338–343 and high crystalline epitaxial thin
films,13,49,88,194,238,344–348 as shown in Fig. 17. The electron mobil-
ity gradually decreases with the electron concentration, from
>100 cm2 /V s at n = 1017 cm−3 to 30–50 cm2 /V s at n = 1019 cm−3
to 10 cm2 /V s at n = 5 × 1020 cm−3 . This indicates that the ion-
ized dopants act as scattering centers.134,170,174 In the case of layers
of poor structural quality, e.g., thin films grown on Al2 O3 sub-
strates with a large mismatch, the electron mobility is much lower
as compared with bulk crystals or with high quality homoepi-
taxial layers because of the scattering at the grain boundaries or
dislocations.173,188,258
In general, a much higher conductivity and carrier concen-
tration have been achieved in epitaxial thin films than in bulk
crystals. Baldini et al.238 achieved a conductivity of 641 S cm−1
in Si doped β-Ga2 O3 grown by MOCVD with a carrier concen-
tration of 8 × 1019 cm−3 and a mobility of 50 cm2 /V s; Ahmadi
et al.13 using MBE achieved a mobility of 39 cm2 /V s and n of
1 × 1020 cm−3 , yielding a conductivity of 625 S cm−1 in Sn doped
Ga2 O3 . Recently, Leedy et al.173 achieved a record-high conductiv-
ity of 732 S cm−1 with a carrier concentration of 1.74 × 1020 cm−3
and mobility of 26.5 cm2 /V s by homoepitaxially growing Si
doped Ga2 O3 films on (010) β-Ga2 O3 substrates using PLD.
The growth of highly conductive doped Ga2 O3 layers has impor-
tant implications for device application. In particular, Ohmic con-
tact formation to wide semiconductors has been a known problem
in Ga2 O3 . The highly conductive Ga2 O3 layers can be used as elec-
trodes to form Ohmic contacts with a low contact resistance.173
Furthermore, because of the large bandgap, the doped Ga2 O3 is
also highly transparent in the visible region, of particular interest
as an alternative to Sn doped In2 O3 (ITO) transparent electrodes in
optoelectronic applications.
1. Activation energies (Ea ) of the shallow donors
Temperature dependent transport measurements, EPR, and
theoretical calculation have also been performed to examine energy
levels of the shallow donors in Ga2 O3 . These results, in general,
revealed a low activation energy (Ea ) of less than 70 meV. However,
some discrepancies still remain regarding the values of Ea and the
exact activation mechanisms;298,272,318 Ea for Sn ranges from 7.4 meV
to 60 meV,331,332 for Si ranges from 16 meV to 50 meV,237,278,299,305,333
and for Ge ranges from 17.5 meV to 30 meV.334,335 The variation
in Ea may be associated with differences in doping concentrations,
other impurities and defects, growth methods, accuracy in the mea-
surements, etc. Recent EPR studies by Son et al.333 reported that
Si may also behave as a negative-U center (often called a DX cen-
ter) with the negative charge state DX− , similar to the Si donor in
Alx Ga1−x N with a high Al content.349 Ea for DX− is in the range
of 44 meV–49 meV. After annealing at 1150 ○ C in nitrogen, the
DX− donors are fully activated and become partly delocalized, form-
ing impurity bands, which reduces the donor activation energy to
Ea = 17 meV. The DX properties and the formation of impurity
bands explain the large variation of the donor activation energies

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reported in the literature. However, other groups have reported
no evidence supporting the DX state.272 Recently, Neal et al.272
performed temperature dependent carrier density and mobility of
n-type β-Ga2 O3 , as determined by Hall effect measurements in van
der Pauw geometry. They accurately determined the donor energy
by reliable estimation of the compensating acceptor concentration
through fitting of the low temperature ionized impurity limited
mobility. Their results indicate that Si and Ge act as typical shallow
donors in β-Ga2 O3 with an ionization energy of 30 meV, as opposed
to shallow DX centers.
Other studies reported relatively deeper donor states. For
example, Neal et al.278 found that the energy level for unintentional
donors with a concentration of ∼1016 cm−3 in commercial Ga2 O3
(2̄01) substrates was measured to be 110 meV using temperature
dependent Hall effect measurements and 131 meV using admittance
spectroscopy. Feng et al.134 grew Si doped (010) β-Ga2 O3 homoepi-
taxial films using MOCVD with a record room temperature mobility
of 184 cm2 /V s; in their film, in addition to the primary shallow
donor state with an activation energy of 34.9 meV and a concentra-
tion of 2.7 × 1016 cm−3 , a secondary deep donor state with an acti-
vation energy of 120 meV and a concentration of 5 × 1015 cm−3 was
also found. Possible origins of the deep donor state at 120 meV could
include antisites, interstitials, and impurities such as hydrogen or Si
APL Mater. 8, 020906 (2020); doi: 10.1063/1.5142999
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FIG. 17. Inverse relationship between n-
type carrier (electron) concentration and
room temperature Hall mobility for (a)
bulk single crystals and (b) high crys-
talline epitaxial thin films [(b) adapted for
Ref. 455].
on the Oh coordinated Ga2 site. The presence of such relatively deep
donors and their ionization percentage at device operating tempera-
tures could have an effect on the on-state resistance and breakdown
voltage of rectifiers.278
While the achievement of highly conductive doped Ga2 O3 is
interesting on the one hand, the achievement of Ga2 O3 bulk crys-
tals and particularly thin films with high carrier mobility and low
defect density, on the other hand, is more crucial for FETs and RF
rectifiers.274,275 As reported by Ma et al.,237 the mobility in Ga2 O3
is limited at 220 cm2 /V s by polar optical phonon (POP) scatter-
ing when the electron concentration is lower than 1 × 1018 cm−3
and by ionized impurity scattering at high electron concentrations.
Great efforts have been made to grow high crystalline quality and
high mobility Ga2 O3 by minimizing the defect, dopant, and carrier
concentration.
Table II shows a summary of the room-temperature mobil-
ity vs carrier concentration for the state-of-the-art doped β-Ga2 O3
bulk single crystals and epitaxial thin films reported in the litera-
ture. It can be seen that the room temperature mobility for epi-
taxial thin films with lowest carrier concentration is close to the
predicted theoretical limit of approximately 220 cm2 /V s. Remark-
ably, Feng et al.134 have recently grown high purity and high
quality (010) β-Ga2 O3 homoepitaxial thin films with controllable
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Si doping as low as 1016 cm−3 using MOCVD. The films were found
to exhibit record-high carrier mobilities of 184 cm2 /V s at room
temperature and 4984 cm2 /V s at 45 K. The extracted compensa-
tion concentration was as low as 9.4 × 1014 cm−3 , which is criti-
cal for controllable tuning of the doping concentration lower than
mid-1015 cm−3 . The Ga2 O3 films grown with high mobility and
low compensation concentration are critical for developing high-
performance lateral and vertical power devices with high critical
fields. Another strategy to achieve high mobility is to use modulation
doped β-(Alx Ga1−x )2 O3 /β-Ga2 O3 heterostructures to form a 2DEG
at the interface. This is attributed to the spatial separation between
ionized impurities and the 2DEG. The high mobility values allowed
for the observations of the Shubnikov–de Haas (SdH) effect oscilla-
tions at cryogenic temperatures.50 A record-high room-temperature
channel mobility of 180 cm2 /V s and a low temperature peak mobil-
ity of 2790 cm2 /V s have recently been demonstrated.50 Both the
mobilities exceeded the highest experimental mobility values for
bulk β-Ga2 O3 .
Doping of Ga2 O3 with transition metals (Nb,269 Ta,270 W,350
Mo, Fe,352 Co,353 and Cr354 ) or rare-earth metals (Eu355 and Er354 )
351
has also received much interest. This is because, on the one hand,
transition metals (e.g., Nb5+ , Ta5+ , W6+ , and Mo6+ ) have higher
oxidization states and, in principle, each dopant donates more elec-
trons than Si and Sn, minimizing scattering by ionized dopants in
order to achieve the same level of carrier concentration. This has
been demonstrated by the achievement of high mobility and con-
ductivity of W356,357 and Mo358,359 doped In2 O3 and Ta360 doped
SnO2 . One the other hand, transition metal doping (e.g., Co) may
be of interest to achieve dilute magnetic semiconductors/oxides,
and rare-earth metals (Eu) could improve the luminescence and
electroluminescence properties.355
Peelaers and Van de Walle361 have performed DFT calculations
on the viability of W, Mo, Re, and Nb as n-type dopants in Ga2 O3 .
Their results show that Nb is the best candidate because it has a low
formation energy (1.19 eV for T d Ga1 at the CBM and 0.31 eV for Oh
Ga2) and a small ionization energy (0.03 eV for T d Ga1 or 0.15 eV
for Oh Ga2 below the CBM), whereas W, Mo, and Re act as deep
donors. Zhou et al.269 have grown high quality β-Ga2 O3 bulk crys-
tals with controllable Nb doping concentration by the OFZ method.
It was proved that Nb is an effective n-type dopant for Ga2 O3 , and
the carrier concentration can be controlled from 9.55 × 1016 cm−3 to
1.8 × 1019 cm−3 by tuning Nb doping concentration. Moderate elec-
trical conductivity and mobility have also been achieved for Zr270
and Ta362 doping in Ga2 O3 bulk crystals. More experimental works
should be done to explore the possibility of other transition metal
dopants.
D. P -type doping in Ga2 O3
As mentioned earlier, p-type doping in wide bandgap oxide
semiconductors including Ga2 O3 remains an outstanding chal-
lenge.363,364 The challenge is due to the intrinsic electronic structure
of oxide semiconductors; (i) the top of VB of most oxides mainly
consists of strongly localized O 2p-derived orbitals, resulting in a
large hole effective mass and, thus, low hole mobility; this means
that most of the doped holes tend to be trapped by local lattices
as small polarons, as opposed to the free holes that are delocal-
ized in the valence band as in conventional semiconductors; (ii) the
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valence bands are deep in energy, and holes are easily compensated
by defects such as Vo, leading to the low p-type dopability, and there-
fore, a shallow acceptor that can contribute to significant hole con-
centrations is still lacking. In simple chemical terms, p-type doping
involves the introduction of holes into the O 2p states at VBM (i.e.,
oxidation of O anions), resulting in strongly localized, deep lying
holes centered on single oxygen sites.
There are limited experimental works on the p-type doping of
Ga2 O3 . Inspired by the success in GaN, Mg doping has received
much attention, but the results are not conclusive. Chikoidze
et al.365 claimed the success of p-type conduction in Mg doped
Ga2 O3 , as proved by combined Hall and Seebeck measurements,
and photoemission and cathodoluminescence spectroscopies, but
the ionization energy of the acceptor level was measured to be
1.1 eV above the VBM. Another study claimed p-type conductiv-
ity in Mg doped Ga2 O3 , but the as-grown materials were highly
resistive, without hole carrier concentration and acceptor ionization
energy being determined.366 Other studies have found that Mg dop-
ing leads to semi-insulating Ga2 O3 367 and gave rise to sub-bandgap
blue luminescence near 2.9 eV.274 Zn is also a potential candidate
for p-type doping in Ga2 O3 . Feng et al.368 reported the fabrica-
tion of p-type Ga2 O3 nanowires doped with Zn, and the homo-
junction consisting of p-type doped nanowires and n-type Ga2 O3
substrates exhibited rectifying behavior. The cathodoluminescence
spectra study suggests that the ionization energies for Zn doped
Ga2 O3 are 0.25–0.5 eV which is relatively shallow and promising, but
the films remained highly resistive.182,369 Overall, achieving efficient
p-type doping remains elusive. On the other hand, doping of accep-
tor impurities (e.g., Fe or Mg) has been used to reduce the back-
ground electron density in Ga2 O3 , e.g., to create insulating material.
Semi-insulating Fe doped Ga2 O3 substrates are available commer-
cially and are widely used for epitaxial thin film growth and device
fabrication.
Extensive theoretical studies have also been done to under-
stand the microscopic mechanism of p-type doping in Ga2 O3 . Early
studies based on standard DFT calculations reported that Zn could
lead to p-type conductivity.370,371 However, it should be noted that
DFT seriously underestimates the bandgaps and the extent of charge
localization at defects, leading to difficulties in determining acceptor
ionization energies. A later study by Kyrtsos et al.271 using hybrid
functional DFT (which provides a better bandgap description) sug-
gested that Zn and other acceptors (Li and Mg) incorporated at the
Ga sites have ionization energies in excess of 1 eV. The calculation by
Varley et al.372 also predicted that holes in Ga2 O3 can self-trap with
a trapping energy of 0.53 eV, indicating that free holes are unsta-
ble and are spontaneously localized as small polarons. The localized
hole states are consistent with the ultraviolet luminescence observed
in undoped Ga2 O3 crystals.274 EPR studies have also observed that
the holes are trapped at nearest-neighbor oxygen sites of the Mg
acceptors.373
Nitrogen (N) has a similar atomic size as oxygen but has one
less valence electron and a higher 2p orbital than oxygen. N has
been explored as a dopant for other oxides such as ZnO but was
theoretically found to have a large formation energy and ionization
energies in excess of 2 eV374,375 and cannot be an effective p-type
dopant in Ga2 O3 .376 The deep energies of N acceptors are caused
by their defect states. It is found that N can form a variety of com-
plexes with native defects, including Vo and Gai , whose presence in
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N doped Ga2 O3 could compensate any p-type conduction.372 This
result suggests that the observed red-light emission originates from
the recombination of an electron trapped on a donor due to Vo and
a hole trapped on an acceptor due to N doping.377
Very recently, Lyons378 using hybrid DFT examined a large
series of potential elements as acceptors in Ga2 O3 , including N,
group 2 (Be, Mg, Ca, and Sr), and group 12 (Zn and Ca), as shown
in Fig. 18. All the elements are found to exhibit acceptor transition
levels above 1.3 eV. After examining formation energies as a func-
tion of chemical potential, Mg is determined to be the most stable
acceptor species, followed closely by Be.
For summary, so far, there is no solid experimental evidence
showing the achievement of high p-type doping in Ga2 O3 ; theo-
retical studies reach the consensus that the conventional acceptor
doping approach gives rise to strongly localized hole states with
larger ionization energies, prohibiting p-type conductivity. This is
inherently caused by the localized nature of the O 2p-derived VB
that leads to difficulty in introducing shallow acceptors and large
hole effective mass. Learning from the design of p-type oxides,379
a way to mitigate this problem is to use the hybridization of O 2p
orbitals with closed-shell Cu 3d10 orbitals and post-transition metal
cations with filled lone pair states (ns2 ), such as Sn2+ (5s2 ) and Bi3+
(6s2 ).363,380,381 For example, because the s orbitals are generally spa-
tially extended, it is, therefore, expected that their hybridization with
O 2p states can result in lower effective mass. Sn in SnO382,383 and
Bi in Ba2 BiTaO6 384 have been proved to lead to a relatively high p-
type mobility. Similarly, Sabino et al.385 proposed based on hybrid
DFT calculation that Bi doped Ga2 O3 , i.e., (Ga1−x Bix )2 O3 solid solu-
tion, introduces a fully occupied intermediate VB that is significantly
higher in energy than the original VB. This intermediate VB is com-
posed mainly of Bi 6s and O 2p orbitals, providing the opportunity to
achieve p-type doping in this system. It would be interesting to carry
out experiments to prove this concept based on high-quality bulk
crystal or thin films. Alternatively, Islam et al.387 recently claimed
that a remarkable hole density of 1020 cm−3 can be achieved by
incorporation of hydrogen at Ga vacancy position in the Ga2 O3 lat-
tice. The hydrogen induced acceptor ionization energy is as low as
42 meV.
Very recently, Chikoidze et al.386 reported an exciting result of
the achievement of a hole mobility of 10 cm2 V−1 s−1 and free hole
concentrations of 1017 cm−3 by annealing Ga2 O3 in oxygen atmo-
sphere. The authors claimed that although p-type doping in Ga2 O3
has been considered impossible due to the flat VB resulting in a
high hole effective mass, it has been also recently reported that the
APL Mater. 8, 020906 (2020); doi: 10.1063/1.5142999
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FIG. 18. Transition levels for group 5 (N),
group 2 (Be, Mg, Ca, and Sr), and group
12 (Zn and Ca) acceptors in Ga2 O3 .
Each center exhibits two transition lev-
els: the (0/−) acceptor transition level
and the deep (+/0) donor level. Results
are presented for N on each unique O
site and for the cation impurities on the
two unique Ga sites.378
hole effective mass in Ga2 O3 is, indeed, fairly anisotropic and can
be as low as 0.4 me for certain crystal orientations. It is particularly
exciting to the research community that p-type Ga2 O3 is possible at
least along some crystal directions. However, more research must
be conducted to verify and determine its prospects for Ga2 O3 solar
blind bipolar optoelectronics and high-power electronics based on
p-n homojunctions.
On the other hand, as long as p-type Ga2 O3 remains elusive,
combining n-type Ga2 O3 with existing wide bandgap p-type semi-
conductors such as p-GaN, SnO, NiO, Cu2 O, Ir2 O3 , CuI, SiC, and
diamond to form p-n heterojunctions would also be a compro-
mising solution for vertical devices. Combining n-type Ga2 O3 with
existing p-type GaN is promising for enabling next-generation high-
performance transistors and optoelectronic devices. Attempts have
been made to grow Ga2 O3 on GaN epi-layers388,389 and directly
grow GaN epitaxially on a Ga2 O3 single crystal substrate10,39,40,390
for the fabrication of a high-responsivity UV photodetector. How-
ever, efforts need to be done to control the interface because of
the incompatible growth of oxides and nitrides.391,392 Diamond is
also a particularly attractive candidate due to its range of highly
desirable properties for power electronics including an ultra-wide
bandgap of 5.5 eV, highest thermal conductivity, high electron and
hole mobilities, and a high electric breakdown field.393 P-type doping
in diamond can be achieved either through conventional substitu-
tional doping with boron (hole mobility of 2000 cm2 /V s)394 or by
inducing on its surface through the so-called surface transfer doping
process (hole mobility of 100–300 cm2 /V s).395 However, the growth
of Ga2 O3 on diamond or vice versa poses a challenge. Integrating
Ga2 O3 with p-type wide bandgap oxides would ease the growth, but
p-type oxides are also limited by their low mobilities, with reported
values of 5–10 cm2 /V s for SnO (optical bandgap of 2.7 eV),381,396–399
divergent values of 0.1–30 cm2 /V s for NiO (optical bandgap of
3.75 eV),400–403 and a reported value of 1 cm2 /V s for Ir2 O3 (optical
bandgap of 2.6 eV).404,405
V. ALLOYING AND BANDGAP ENGINEERING
WITH Al2 O3 AND In2 O3
Over the past decades, tremendous progress has been made
in the engineering of the bandgaps of semiconductors over a wide
range by tuning the composition of semiconductor alloys that have
the same crystal structure and similar lattice constants, as shown in
Fig. 19. For example, the bandgaps of Inx Ga1−x N and Aly Ga1−y N can
be systematically tuned from 1.9 eV to 3.5 eV by varying the x value
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FIG. 19. Relationship between bandgap and bond length for various compound
semiconductors including several extensively investigated semiconductor alloying
systems.456
and from 3.5 eV to 6.28 eV by varying the y value, respectively.406
Extensive understanding of material properties and continued pur-
suit of high-quality thin film growth lead to various optimized het-
erostructures and superlattices and, consequently, the rapid estab-
lishment of high performance III-nitride-based optoelectronics. In a
similar fashion, there is also possibility to use Al2 O3 (Eg = 8.8 eV),
Ga2 O3 (Eg ∼ 4.8 eV), and In2 O3 (Eg = 2.9 eV) to design ternary
or quaternary alloys. Alloying Ga2 O3 with Al2 O3 and In2 O3 would
offer an opportunity to tailor the bandgaps and other properties
and to form heterojunctions, enabling electronic modulation and
confinement. However, a major problem is that Al2 O3 , Ga2 O3 , and
In2 O3 have quite different crystal structures. It is, therefore, interest-
ing to understand which crystal structure the alloys would adopt and
how their structures affect the optical and electronic properties. In
the following, we first provide a brief introduction on the structures
and properties of each oxide.
A. Crystal structures
Al2 O3 crystallizes in a corundum structure (space group R3̄c)
with lattice constants of a = 4.76 Å and c = 12.99 Å, as shown
in Fig. 20(a). This structure is based on a hexagonally close
packed array of O ions with the Al cations filling up 2/3 of the
central Oh sites. Al2 O3 is the commonly used substrate for the
growth of GaN and Ga2 O3 . The bandgap of Al2 O3 is 8.8 eV.
Al2 O3 also has a metastable monoclinic structure, same as β-phase
of Ga2 O3 .
The thermodynamically stable phase of In2 O3 adopts a body-
centered cubic (bcc) bixbyite structure, with a lattice parameter of
a = 10.117 Å.407 The structure may be regarded as a 2 × 2 × 2
APL Mater. 8, 020906 (2020); doi: 10.1063/1.5142999
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FIG. 20. (a) Corundum structure of Al2 O3 and (b) bixbyite structure of In2 O3 .
superstructure of fluorite with ordered removal of O from 1/4
of the anion sites, as shown in Fig. 20(b). In3+ cations are Oh
coordinated by six O anions but with slightly different bond-
ing lengths. The bixbyite In2 O3 has a fundamental bandgap of
2.9 eV but is optically forbidden; the optical bandgap with a strong
absorption occurs at 3.75 eV.284 In2 O3 is also a metastable poly-
morph of hexagonal corundum structure, with a lattice constant of
a = 5.478 Å and c = 14.51 Å. The corundum phase In2 O3 has a direct
bandgap of 3.0 eV.408 Although the corundum In2 O3 is a metastable
phase, it has been shown that it can be stabilized at the interface
during the epitaxial growth of In2 O3 on Al2 O3 substrates.409
As mentioned earlier, Ga2 O3 adopts five polymorphs. The
monoclinic β-Ga2 O3 is the most stable one. In β-Ga2 O3 , Ga has
a Td coordinated Ga1 site and Oh coordinated Ga2 site. α-Ga2 O3
is equivalent to the corundum structure with lattice constants of
a = 4.76 Å and c = 12.99 Å. In the corundum phase, only Oh
coordinated sites are present. γ-Ga2 O3 is equivalent to the bixbyite
structure with a = 8.22 Å.
B. (Alx Ga1−x )2 O3
Al2 O3 alloyed with Ga2 O3 , i.e., (Alx Ga1−x )2 O3 , in principle, can
increase the bandgap from 4.85 eV to 8.8 eV. However, as men-
tioned above, different crystal structures and coordination bring
frustration as for what is the preferred crystal structure as a func-
tion of x. For the bulk polycrystallines prepared by solid state
synthesis254 and thin films grown by PLD,230,253 it was reported
that (Alx Ga1−x )2 O3 keep the monoclinic β-phase with Al contents
up to x = 0.80.410 With more Al content, the corundum struc-
ture is preferred. However, it should be noted that for the epitax-
ial thin films using MBE, the solubility of Al in (Alx Ga1−x )2 O3 is
restricted to x = 0.20.51 The limited Al contents were attributed to
the low growth temperature (<800 ○ C) during MBE growth, while
incorporation of Al in Ga2 O3 lattice requires a temperature higher
than 800 ○ C.88,150
The lattice constants decrease linearly with an increase in the
Al-content, consistent with the smaller atomic radius of Al com-
pared to Ga. The linear decrease in lattice constant is in agreement
with Vegard’s law. The recent DFT calculations by Peelaers et al.410
revealed more insights into the phase stabilities, lattice parame-
ters, and electronic properties of (Alx Ga1−x )2 O3 alloys. They found
that the monoclinic phase remains energetically preferable for Al
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concentrations up to x = 0.71; for a higher Al content, a corun-
dum structure is preferred, in close agreement with experimental
phase diagrams.230,253,254 More interestingly, it was found that the
energetics strongly correlate with the preferred coordination envi-
ronment of Al and Ga: Al atoms favor Oh sites, which are the
only coordination environments in corundum; in the monoclinic
structure, half of the sites are Oh coordinated and half of the sites
are T d coordinated. Therefore, the x = 0.5 alloy (GaAlO3 ) has a
high stability with all Al atoms at the Oh sites and all Ga atoms at
T d sites.
As, expected, the bandgaps of (Alx Ga1−x )2 O3 alloys can be
tuned from the bandgap of β-Ga2 O3 (4.8 eV) to 6 eV with an
increase in Al contents. Figure 21(b) shows the experimentally
measured and DFT calculated bandgaps for the monoclinic and
corundum (Alx Ga1−x )2 O3 as a function of Al contents, adapted
from Ref. 411. Good agreement is found between the calculated
and experimental values.410 The increased bandgaps would enable
the realization of new applications in many devices such as FET,
modulation-doped electron channels, and solar-blind photodetec-
tors responsive to deeper UV bands.412 For example, the larger
bandgap of β-(Alx Ga1−x )2 O3 would lead to an even higher BFOM
than that of Ga2 O3 , which makes β-(Alx Ga1−x )2 O3 a potential
candidate for even higher power and higher frequency electronic
devices. Kaun et al.51 have grown (Alx Ga1−x )2 O3 epitaxial thin
films using MBE with composition up to x = 0.2. A prelimi-
nary report on β-(Alx Ga1−x )2 O3 MESFETs shows a higher crit-
ical breakdown field than β-Ga2 O3 .413 However, a low mobility
of 4 cm2 /V s in the grown β-(Alx Ga1−x )2 O3 film results in a
lower on-current in the device. Further work needs to be done to
improve the crystal quality and mobility. Another very interesting
use of β-(Alx Ga1−x )2 O3 is as a barrier layer for β-(Alx Ga1−x )2 O3 /β-
Ga2 O3 high electron mobility transistors (HEMTs). β-Ga2 O3 suf-
fers from POP scattering which limits its maximum mobility to
220 cm2 /V s.237 Because of the larger bandgap of β-(Alx Ga1−x )2 O3 ,
i.e., higher CBM, it is expected that electrons in (Alx Ga1−x )2 O3
doped by Si would be transferred to the adjacent Ga2 O3 to form a
2DEG at the interface. The enhanced 2DEG sheet charge is predicted
to screen out certain phonon modes, resulting in reduced scatter-
ing in the 2DEG channel. Theoretical studies predict that the 2DEG
at the β-(Alx Ga1−x )2 O3 /β-Ga2 O3 interface has a mobility of about
500 cm2 /V s,414 much higher than that of bulk β-Ga2 O3 . Recently,
modulation-doped β-(Alx Ga1−x )2 O3 /β-Ga2 O3 HEMTs with a sheet
charge of 2 × 1012 cm−2 and Hall mobility of 180 cm2 /V s have been
demonstrated.50
C. (Inx Ga1−x )2 O3
While there is extensive research work in (Alx Ga1−x )2 O3 alloys,
the literature on (Inx Ga1−x )2 O3 ternary alloys is limited. In2 O3
(doped with 6% Sn, known as ITO) has been extensively investi-
gated as a transparent electrode for flat panel displays, touch screens,
and solar cells. The bandgap of In2 O3 has been widely quoted to
be 3.75 eV,415,416 which marks the onset of strong optical absorp-
tion. A weaker absorption onset at 2.62 eV has either been ignored
or been attributed to indirect optical transitions.417 In 2008, it was
established based on XPS and DFT that In2 O3 has a direct but
optically forbidden bandgap of around 2.9 eV.284 The establish-
ment of fundamental bandgap in turn leads to the identification
of the surface electronic structure of In2 O3 , e.g., strong downward
band bending and 2DEG at the surface of In2 O3 .418–421 Alloying
Ga2 O3 with In2 O3 offers the opportunity to tune the bandgaps from
4.8 eV to a lower value (2.9 eV) and also other material proper-
ties. However, similar to the (Alx Ga1−x )2 O3 system, because Ga2 O3
and In2 O3 have quite different crystal structures, phase separation
is expected. Shannon and Prewitt investigated the structural prop-
erties of (Inx Ga1−x )2 O3 powder and single crystalline samples for
0 < x ≤ 0.5422 and found that a monoclinic β-phase structure was
maintained. A complete phase diagram of (Inx Ga1−x )2 O3 alloys was
established by Edwards et al.,423 using powder samples prepared by
conventional solid state synthesis; they showed that the solubility
of In2 O3 in Ga2 O3 maintaining a monoclinic structure is limited
at x = 0.44, while on the In2 O3 side, the solubility limit for Ga in

FIG. 21. Lattice parameter and bandgap evolutions as a function of Al contents in (Alx Ga1−x )2 O3 alloy contents. (a) Pseudocubic lattice parameter as a function of alloy
composition x for the corundum and monoclinic structures. Experimental values for monoclinic are shown as solid black triangles, open triangles, and solid downward
triangles. The top inset shows the monoclinic unit cell, and the bottom inset shows the corundum unit cell. Octahedrally coordinated sites are indicated in blue, and
tetrahedrally coordinated sites are indicated in green. Small red spheres depict O atoms. (b) Direct (solid symbols) and indirect (open symbols) bandgaps for the monoclinic
and corundum structures as a function of the alloy composition. The solid (dashed) lines are quadratic fits to the indirect (direct) bandgaps, as described in the text. The
computed values are shown in color, and the experimental values are shown in black.411

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the cubic bixbyite phase is only at (1 − x) = 0.1. In the composi-
tion range between the two doping limits, bulk samples are biphasic,
consisting of a mixture of cubic Ga doped In2 O3 and monoclinic
In doped β-Ga2 O3 . Most of the works also found that the lattice
constants of (Inx Ga1−x )2 O3 increase linearly with an increase in the
In content,424–426 as expected from the larger cation size of In3+
(0.79 Å) as compared to Ga3+ (0.62 Å). As shown in Fig. 22(a),
the increase in lattice parameters (a, b, c) is in agreement with
Vegard’s law.
Epitaxial (Inx Ga1−x )2 O3 thin films have been prepared by a
wide range of techniques including MBE,425 MOCVD,159 PLD,427–429
and so on, but the reported solubility values are quite scat-
tered depending on the growth techniques and growth condi-
tions. Oshima and Fujita425 grew β-(Inx Ga1−x )2 O3 thin films on
β-Ga2 O3 buffer layers on Al2 O3 (0001). The thin films had a mon-
oclinic structure up to x = 0.35; the crystalline quality degraded
with an increase in the In content such that films with x = 0.35
were nearly amorphous. MOCVD thin films on Al2 O3 (0001) crys-
tallize in the monoclinic structure for x ≤ 0.22. For x ≥ 0.51,
only the cubic structure of In2 O3 is observed. Kokubun et al.430
prepared (Inx Ga1−x )2 O3 thin films on Al2 O3 (0001) by a sol-gel
method. For x < 0.4, the monoclinic structure was observed,
while for x > 0.8, the bixbyite structure was observed. For inter-
mediate x values, the monoclinic and the cubic phase coexist.
Baldini et al.159 grew monoclinic (Inx Ga1−x )2 O33 thin films by
MOVPE for x ≤ 0.25, while for higher In admixture, phase sep-
aration occurred. UV and deep-UV selective photodiodes from
visible-blind to solar-blind were realized based on a Si-doped
(Inx Ga1−x )2 O3 thin film with a monotonic lateral variation of
0.0035 < x < 0.83.431
First-principle calculations were also performed to reveal more
insights into the formation enthalpies, structural parameters, and
electronic properties of the alloys. Maccioni and Fiorentini432
showed that the solubility limit of In in Ga2 O3 was x = 0.1, sig-
nificantly lower than the experimentally derived values of 0.43.
Recently, Peelaers et al.433 showed that a monoclinic phase is ener-
getically favorable for x < 0.5. All In cations prefer occupying the
Oh sites because of their much larger size than that of Ga. In incor-
poration increases the local strain around the In cations, resulting
APL Mater. 8, 020906 (2020); doi: 10.1063/1.5142999
© Author(s) 2020
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in phase instability at higher In contents. A lower In content results
in a partial occupation of the Oh sites by Ga atoms. This effect
may explain why the cation ordered GaInO3 with all In at the
Oh sites and all Ga at T d sites similar to the case of GaAlO3
were rarely synthesized and perhaps can only be synthesized at
high pressures.
The incorporation of In in Ga2 O3 allows us to tailor the
optical bandgap from 4.86 eV down to 4.1 eV in the range of
x = 0–0.44. Thin films grown by the MBE,425 MOCVD,159 PLD,427,428
and sol-gel method430 have been measured using optical absorp-
tion spectroscopy. Figure 22(b) presents a few typical results from
Refs. 13, 49, 170, 194, 238, 347, and 434. The bandgaps systemat-
ically decrease with an increase in the In content.435 For x ≤ 0.3,
the absorption edge depends linearly on x and can be fitted by
Eg (x) = 4.90 eV − (2.42 × x) eV. Although the bandgaps have been
deduced from optical absorption edges for higher x values (x > 0.44),
bandgap bowing can be observed and can be fitted by Eg (x) = 4.87 eV
− (2.16 × x) eV + (1 × x2 ) eV for 0 < x < 1. However, it should
be noted compositions for 0.44 < x < 0.90 produce mixed phases
of β-GaInO3 and bixbyite InGaO3 . Furthermore, In2 O3 actually has
a much smaller fundamental bandgap (2.9 eV) than the optical
bandgap (3.7 eV).284
Finally, it is interesting to note that the α-phase Ga2 O3
has the same corundum structure as Al2 O3 . All Ga cations are
Oh surrounded by six oxygen ions. The lattice parameters are
a = 4.9825 Å and c = 13.433 Å.82 Epitaxial thin films of α-Ga2 O3
can be stabilized by growing on α-Al2 O3 by mist-CVD at
430–470 ○ C.83,172,245 The stabilization of the α-phase was attributed
to the unique reaction path of this growth technique. The incor-
poration of Al contents up to 0.81 was reported by Ito et al.171
The bandgap was increased from 5.3 eV to 7.8 eV. The ther-
mal stability of the α phase is strongly enhanced due to alloying
with α-Al2 O3 .
Moreover, the metastable corundum phase In2 O3 has the same
corundum structure as α-phase Ga2 O3 . It has been shown that
corundum In2 O3 could be stabilized by the Al2 O3 409 or Fe2 O3 buffer
layer on Al2 O3 .436 In the α-(Inx Ga1−x )2 O3 alloy system, a phase
separation occurs for intermediate In admixtures. In Fig. 23, the
bandgap energy of the experimentally realized solid solutions of
FIG. 22. (a) Lattice parameters for
(Inx Ga1−x )2 O3 samples as a function of
In concentration. Data from bulk pow-
ders, thin film samples, and ceramic
samples are shown in black squares,
blue squares, and red triangles, respec-
tively.457 (b) Bandgap energy of (Ga,
In)2 O3 bulk crystals and thin films deter-
mined from absorption measurements.
The dotted black line and the dashed
black line are calculated values. The rest
of the results are obtained experimen-
tally. The black line is a fit to the exper-
imental data excluding results for E//b
and that of Fujita et al. See Ref. 458 for
more details.
8, 020906-22
 APL Materials
FIG. 23. Bandgap energy in terms of averaged bond length and a-axis lat-
tice constants of experimentally realized solid solutions of α-(Alx Ga1−x )2 O3 and
α-(Inx Ga1−x )2 O3 .437
α-(Ga,In)2 O3 and α-(Ga,Al)2 O3 is shown to depend on the average
bond length and a-lattice constant. The dependence of the bandgap
energy on the composition can be fitted by Eg (x) = xEg(α-Ga2O3)
+ (1 − x)Eg(Al or In) − bx(1 − x), with Eg(Al or In) being the bandgap
of α-Al2 O3 or α-In2 O3 with the respective bowing parameters of
b = 0.1 eV or b = 1.1 eV.437 Furthermore, there are a variety of rhom-
bohedral corundum-structured M2 O3 oxides, including M = Al, Ga,
In, Cr, Fe, and V. Owing to the same crystal structure, alloying
and the formation of heterostructures with α-Ga2 O3 and α-In2 O3
are essentially expected, leading to novel multi-functionality, such
as a wide range tunability in the bandgap and ferromagnetic semi-
conducting properties (e.g., weak ferromagnetic Fe2 O3 87,436 with a
bandgap of 2.2 eV).
Motivated by the successful epitaxial growth of ε-Ga2 O3 as well
as κ-Ga2 O3 , Al and In alloying of these two unstable phases begins
to come into the view of researchers.438–441 Tahara et al.438 first
reported the Al2 O3 alloying in ε-Ga2 O3 using mist-CVD, with the Al
content of ε-(Alx Ga1−x )2 O3 reaching up to the value of x = 0.395 and
bandgap tuned from 5.0 eV to 5.9 eV. In2 O3 alloying with ε-Ga2 O3
was also achieved by mist-CVD, and its bandgap could be controlled
from 4.5 eV to 5.0 eV without phase separation.439 Recently, alloy-
ing in κ-Ga2 O3 was reported by the researchers from Universität
Leipzig.440–442 A specially designed continuous composition spread
(CCS)-PLD method was utilized to grow κ phase (Alx Ga1−x )2 O3 and
(Inx Ga1−x )2 O3 . For Al alloying, the Al content could be achieved
to a remarkable value of x = 0.65 with a tunable bandgap value
from 4.9 eV to 5.8 eV.440 The In alloying was reported with a
maximum content of x = 0.35 and the bandgap value varied from
4.3 eV to 4.9 eV.442
APL Mater. 8, 020906 (2020); doi: 10.1063/1.5142999
© Author(s) 2020
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VI. SUMMARY AND REMARKS
In this article, we provided a timely review on the semiconduc-
tor physics of Ga2 O3 in terms of electronic structures, optical prop-
erties, chemistry of defects and dopants, and bandgap engineering.
Recent progress and fundamental understanding on the synthesis
of bulk single crystals, epitaxial growth of thin films, chemical and
physical properties of defects and impurities, deep level states, and
origin of unintentional n-type doping, p-type doping, and ternary
alloys with In2 O3 and Al2 O3 were reviewed.
In the past decade, a significant process has been made for
the growth of high-quality bulk crystals and thin films of Ga2 O3 .
4-in. high quality β-Ga2 O3 (2̄01) wafers grown by EFG with EPD
on the order of 103 cm−2 were commercially available from Novel
Crystal Technology, Inc. High quality β-Ga2 O3 homoepitaxial thin
films, with record-high carrier mobilities of 184 cm2 /V s and low
carrier concentrations of 2.5 × 1016 cm−3 , have been achieved by
MOCVD.134 This enables further scaling-up for mass production.
Using Si, Sn, or Ge as dopants, electron carrier concentrations rang-
ing from 1016 up to 1020 cm−3 can be controllably obtained.13,49
Through modulation doped β-(Alx Ga1−x )2 O3 /Ga2 O3 heterostruc-
tures to form a two-dimensional electron gas at the interface, a
record-high room-temperature channel mobility of 180 cm2 /V s
and peak mobility of 2790 cm2 /V s at 50 K have also been
demonstrated.50
The achievement in growing high quality bulk crystals and thin
films has accelerated research progress in the fundamental under-
standing of semiconductor physics of Ga2 O3 and device optimiza-
tions. Similar to other oxide semiconductors such as ZnO, In2 O3 ,
and SnO2 , Ga2 O3 exhibits unintentional n-type conductivity. The
origin of the unintentional doping is still not clear. VO , Hi , HO ,
Gai , and impurities from the synthesis/growth processes have been
proposed as possible sources. Based on more advanced hybrid DFT
calculations and evidence from experiments, it appears that Vo is a
deep level donor, unlikely contributing free electrons at room tem-
perature, and Gai has a high formation energy. Hydrogen and unin-
tentional impurities such as Si are most likely the origins of unin-
tentional n-type conductivity. Several studies reported the detection
of Si residual (with ppm wt) even in 6N purity Ga2 O3 . Such a trace
amount of Si can lead to a free electron density of ∼1016 cm−3 . Fur-
thermore, a trace amount of Fe impurity has also been detected in
bulk crystals likely from the containers used for material growth.
It is interesting to obtain Ga2 O3 precursors with an even higher
purity, thus eliminating possible contaminations during the syn-
thesis process to further reduce the background electron carriers.
Several deep level states, including E1 (EC -0.62 eV), E2 (EC -0.82 eV),
E3 (EC -1.00 eV), E4 (EC -2.16 eV), and E5 (EC -4.4 eV), have been
detected in bulk single crystals and epitaxial thin films. These deep
level states may be associated with the above-mentioned uninten-
tional impurities (e.g., Fe) or defects (e.g., Vo and VGa ) or may be
the intrinsic properties of Ga2 O3 . The identification of their phys-
ical origins is an important task because these deep level states
are associated with the breakdown voltage, specific on-resistance,
and leakage in power electronic devices and may also be associated
with the long delay times and persistent photoconductivity often
observed in solar-blind photodetectors. It has been proved that Si,
Sn, Ge, and Nb act as shallow dopants with activation energy in the
range of 10–60 meV. The doping behaviors (conductivity, carrier
8, 020906-23
 APL Materials
concentration, mobility, activation, Fermi level, optical properties,
etc.) can be understood by classic semiconductor physics. There
are certain discrepancies regarding the electronic structure and sub-
stitution sites of the dopants, e.g., Si substitution at the Ga1 site
may act as deep donors. More experiments based on temperature
dependent transport measurement, EPR, photoluminescence, pho-
toemission, x-ray absorption, and so on should be performed to
clarify this point. It is a challenging task to achieve p-type dop-
ing in Ga2 O3 , which is inherently caused by the localized nature of
the O 2p-derived VBM that leads to difficulty in introducing shal-
low acceptors but the ease of formation of localized polaron states.
So far, there is a lack of strong experimental evidence proving the
achievement of p-type doping in Ga2 O3 . Some new strategies have
been proposed but remain to be further proved, such as to form a
band using elements such as Bi3+ and Sn2+ containing ns2 lone pair
states or hydrogen substitution at the Ga position. One the other
hand, integrating Ga2 O3 with other p-type semiconductors (p-GaN,
SiC, and diamond) or oxides (NiO, Cu2 O, and Ir2 O3 ) to form p-n
heterojunctions would be a convenient solution. In particular, inte-
gration of Ga2 O3 with p-type diamond could open up new opportu-
nities to develop high-performance and robust power devices. Being
the best thermal conductor (thermal conductivity of diamond of
22 W cm−1 K−1 ), diamond can additionally help mitigate the low
thermal conductivity of Ga2 O3 by dissipating heat from it, in a sim-
ilar fashion as GaN-on-diamond power electronics in which dia-
mond acts as a heat spreader.443 However, there remain significant
challenges in the direct growth of one on the other due to lattice
mismatch and different crystal symmetries. Transfer of mechan-
ically exfoliated Ga2 O3 nanomembranes on a diamond substrate
provides an alternative approach to forming van der Waals-type
heterojunctions,444 but this procedure clearly poses limitation to
practical applications.
Despite Ga2 O3 having a small electron effective mass, the Hall
mobility of Ga2 O3 is limited to 220 cm2 /V s due to POP scattering
and decreases with an increase in doping and defects due to ion-
ized impurity scattering.237 Besides the continuous efforts to further
increase the quality of material growth, modulation doping using the
β-(Alx Ga1−x )2 O3 /β-Ga2 O3 interface has been proved as a promising
strategy to enhance the mobility. It is predicted that 2DEG at the
interface can screen out certain phonon modes and a mobility of
∼500 cm2 /V s can be achieved.414
Bandgap engineering by alloying with Al and In results in an
increase or reduction in the bandgap and offers new properties for
the realization of enhanced device performance, such as increased
bandgap for higher power electronic devices, forming heterostruc-
tures for high electron mobility devices and the design of wave-
length selective photodetectors. However, because Al2 O3 , Ga2 O3 ,
and In2 O3 have quite different crystal structures, their ternary alloys
adopt a variety of crystal structures with different solubility lim-
its, which also leads to different optical and electronic properties.
For bulk crystals, (Alx Ga1−x )2 O3 keeps the monoclinic phase with
x up to x = 0.80; a corundum structure is preferred with x > 0.80.
The bandgap of (Alx Ga1−x )2 O3 can be tuned from 4.8 eV to 6 eV.
However, in the epitaxial thin films using MBE, the solubility of Al
in (Alx Ga1−x )2 O3 is restricted to x = 0.20 because the incorpora-
tion of Al in Ga2 O3 requires a higher temperature (>800 ○ C) than
that required for the MBE growth. It was predicted that to avoid
unwanted parallel conduction channels in MODFETs based on
APL Mater. 8, 020906 (2020); doi: 10.1063/1.5142999
© Author(s) 2020
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β-(Alx Ga1−x )2 O3 /β-Ga2 O3 heterostructures and achieve a high per-
formance modulation doping, a large CB offset of at least 0.47 eV is
preferred, which requires a bandgap of 5.15 eV with an Al concen-
tration of x > 0.2.445 Increasing Al contents using other growth tech-
niques (e.g., MOCVD and PLD) and demonstration of modulation
doped devices remain to be explored. Furthermore, the as-grown
β-(Alx Ga1−x )2 O3 films still showed a low mobility of 4 cm2 /V s,
which results in a lower on-current in devices. Further work needs to
be done to improve the crystal quality and carrier mobility. Alloying
Ga2 O3 with In2 O3 has been less explored. In2 O3 in Ga2 O3 maintain-
ing a monoclinic structure is limited at x = 0.44, which allows us to
tailor the optical bandgap from 4.86 eV down to 4.1 eV. This would
offer opportunity to realize selective optoelectronic devices from UV
to deep-UV. Overall, the fundamental research on the alloys is still
in its infancy and the realization of heterostructures and devices still
awaits demonstration.
Finally, it is important to point out that although β-Ga2 O3 has
been extensively studied, α-Ga2 O3 has the potential as the dark horse
in Ga2 O3 research. Although it is a metastable phase, it can be stabi-
lized by Al2 O3 substrates because of the same crystal structures and
the small lattice mismatch. As a matter of fact, the only commer-
cial Ga2 O3 device at present is the SBD fabricated using α-Ga2 O3
grown by mist-CVD and commercialized by FLOSFIA, Inc. In view
of the material structure, α-Ga2 O3 with only Oh coordinated Ga pro-
vides a more symmetric structure to achieve low defect density and
possible higher mobility (300 cm2 /V s). The corundum structure is
more compatible with many other oxides and III-V semiconductors.
α-Ga2 O3 can form solid solutions with Al2 O3 and corundum In2 O3 .
FLOSFIA, Inc. and a group from Kyoto University recently reported
that α-Ga2 O3 can form epitaxial p-n heterojunctions with corundum
Ir2 O3 as an inversion layer.122 Certainly, more attention should be
paid to α-Ga2 O3 .451
ACKNOWLEDGMENTS
K. H. L. Zhang is grateful for funding support from the National
Natural Science Foundation of China (Grant No. 21872116).
D.-C.Q. acknowledges the support of the Australian Research
Council (Grant No. FT160100207) and the continued support
from the Queensland University of Technology (QUT) through
the Centre for Materials Science. L.C. acknowledges the sup-
port from the National Natural Science Foundation of China
(Grant No. 51972160) and the Science and Technology Research
Items of Shenzhen (Grant Nos. JCYJ20170412153325679 and
JCYJ20180504165650580).
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