ECS Journal of Solid State Science and Technology, 2020 9 045004

Ultrawide-Bandgap p-n Heterojunction of Diamond/β-Ga2O3 for a

Solar-Blind Photodiode
Hyun Kim,1 Sergey Tarelkin,2,3,4 Alexander Polyakov,3 Sergey Troschiev,2,4
Sergey Nosukhin,2 Mikhail Kuznetsov,2 and Jihyun Kim1,*,z
1
Department of Chemical and Biological Engineering, Korea University, Anam-dong, Sungbuk-gu, Seoul 136-713 Korea
2
Technological Institute for Superhard and Novel Carbon Materials, Troitsk, Moscow 108840, Russia
3
National University of Science and Technology MISiS, Moscow 194017, Russia
4
The All-Russian Research Institute for Optical and Physical Measurements, Moscow 119361, Russia

The potential of ultrawide-bandgap (UWBG) semiconductors has not been fully explored because of the difficulty of forming a p-n
homojunction. In this study, a mixed-dimensional UWBG p-n heterojunction composed of a p-type diamond substrate and an n-
type exfoliated β-Ga2O3 nanolayer has been demonstrated via a van der Waals interaction; this type of structure does not suffer
from lattice mismatch. Rectifying current-voltage characteristics with a rectification ratio exceeding 107 were obtained with a high
reverse hard breakdown voltage of 135 V. This UWBG p-n heterojunction diode exhibited good thermal stability at elevated
temperatures, retaining its high rectification ratio and low reverse leakage current. Excellent photoresponse characteristics,
including responsivity (12 A W−1), rejection ratio (8.5 × 103), photo-to-dark-current ratio (3900), and fast response/decay
characteristics, were observed from the diamond/β-Ga2O3 p-n heterojunction photodiode, showing no persistent photoconductivity.
The mixed-dimensional p-n heterojunction diode based on two UWBG semiconductors (p-type diamond and n-type β-Ga2O3) can
be used as a robust building block in next-generation power electronics and solar-blind optoelectronics.
© 2020 The Author(s). Published on behalf of The Electrochemical Society by IOP Publishing Limited. This is an open access
article distributed under the terms of the Creative Commons Attribution Non-Commercial No Derivatives 4.0 License (CC BY-
NC-ND, http://creativecommons.org/licenses/by-nc-nd/4.0/), which permits non-commercial reuse, distribution, and reproduction
in any medium, provided the original work is not changed in any way and is properly cited. For permission for commercial reuse,
please email: oa@electrochem.org. [DOI: 10.1149/2162-8777/ab89b8]

Manuscript submitted January 31, 2020; revised manuscript received March 1, 2020. Published April 23, 2020. This paper is part
of the JSS Focus Issue on Gallium Oxide Based Materials and Devices II.
Supplementary material for this article is available online

β-phase gallium oxide (β-Ga2O3) has emerged as a next-
generation ultrawide energy bandgap (UWBG) semiconductor
material owing to its energy bandgap of 4.7–4.9 eV (direct) and its
chemical robustness.1,2 Photodetectors based on β-Ga2O3 enable us
to sense UV-C wavelengths on Earth without interference from
sunlight; this is important for applications in missile tracking, optical
flame detection, and corona detection in high-voltage transmission
and distribution systems. Different types of β-Ga2O3 solar-blind
photodetectors including metal-semiconductor-metal3,4 and photo-
conductive structures5,6 have been reported, exhibiting good selec-
tivity and responsivity to deep UV wavelengths. Lin et al. fabricated
vertical β-Ga2O3 Schottky barrier diodes with a guard ring formed
by nitrogen-ion implantation and achieved a breakdown voltage of
1430 V.7 Tetzner et al. demonstrated a lateral β-Ga2O3 MOSFET
with an 1800 V breakdown voltage and a record power figure-of-
merit of 155 MW cm−2.8 The availability of large crystalline
substrates with controllable carrier concentrations from semi-insu-
lating to n-type is responsible for many of the recent improvements
that will lead to affordable high performance power devices in the
future.
Low-dimensional β-Ga2O3 nanostructures can be obtained by
catalytic growth, catalyst-free growth, and mechanical exfoliation of
the crystalline substrate. Among these, the mechanical exfoliation
method allows the fabrication of freestanding quasi-two-dimensional
nanolayers that retain their electrical and optical properties. The
anisotropy in the lattice constants of β-Ga2O3 (a [100] = 12.225 Å, b
[010] = 3.039 Å, c [001] = 5.801 Å) enables facile cleavage
along the (100) and (001) planes.9 Hwang et al. demonstrated
field-effect transistors based on exfoliated β-Ga2O3 flakes, proposing
β-Ga2O3-based high-voltage nanoelectronics.10 The absence of p-
type doping in β-Ga2O3 is still an issue, and requires forming a
heterostructure with some other p-type semiconductors for fabri-
cating bipolar electronic devices. Shin et al. integrated p-Si with an
exfoliated β-Ga2O3 nanolayer, forming a p-n heterojunction diode.11
*Electrochemical Society Member.
z
E-mail: hyunhyun7@korea.ac.kr
Montes et al. reported a p-n heterojunction by using p-type GaN and
an n-type β-Ga2O3 nanolayer.12 Nakagomi et al. demonstrated n-
type β-Ga2O3/p-type 4H-SiC heterojunctions with high temperature
stability.13 However, the electrical potential of β-Ga2O3 material has
not yet been fully explored because the p-type semiconductors
mentioned above have narrower energy bandgaps than β-Ga2O3.
Diamond semiconductor with an UWBG of 5.46–5.6 eV has
been studied because of its outstanding intrinsic properties such as
high thermal conductivity (>2000 W m−1·K−1), saturation velocity
(>107 cm s−1), and critical breakdown field (10–20 MV cm−1).14,15
High-quality crystalline substrates have been grown by the high-
pressure high-temperature (HPHT) technique. Although the n-
doping of diamond is extremely challenging, the p-doping can be
achieved by the incorporation of boron (relatively deep acceptor
with 0.37 eV).14,16,17 Since its high thermal conductivity can
effectively dissipate the heat generated under high power operation,
the integration of p-type diamond substrates with n-type β-Ga2O3
can be an ideal combination to address the poor thermal conductivity
of β-Ga2O3 (10–30 W m−1·K−1).2 In addition, p-n junction photo-
diodes present fast response time and low dark current because of
their built-in electric field. However, the β-Ga2O3 p-n homojunction
photodiode has not yet been demonstrated because of the absence of
effective acceptors. In our experiments, a p-diamond substrate was
bonded with an exfoliated n-type β-Ga2O3 nanolayer via a van der
Waals interaction, forming a mixed-dimensional UWBG p-n hetero-
junction with a sharp interface.
Experimental
The diamond crystal was grown on a seed at 5.5 GPa/1700 K
using a temperature gradient method,18,19 and doping was realized
by adding 0.5 at% amorphous boron to the growth mixture
(Fe–C–Al–B). The (001) 300 μm-thick substrate was cut by a laser
and mechanically polished on both sides. The p-type diamond
substrate had an acceptor concentration of ∼1019 cm−3, corre-
sponding to ∼1017 cm−3 free holes at room temperature with an
average mobility of ∼50 cm2 V−1·s−1 due to strong scattering by
non-ionized acceptors. Room temperature resistivity was measured
 ECS Journal of Solid State Science and Technology, 2020 9 045004
as 1.5 Ω·cm. Detailed electrical properties of this diamond substrate can
be found in a previous work.20 The back Ohmic contact to the p-
diamond was formed by magnetron sputtering of Ti/Pt/Au (30/10/
100 nm), followed by vacuum annealing at 700 °C. Hydrogen
silsesquioxane (HSQ) electron-beam resist was spin-coated (4500 rpm
for 60 s) on the front surface of the p-diamond as a dielectric to isolate
the metallization of the β-Ga2O3 from the diamond substrate as shown
in Fig. 1a. HSQ was mixed with methyl isobutyl ketone (MIBK) (Dow
Corning FOx-15) to control its thickness, and the spin-coating was
followed by thermal treatment at 200 °C for 2 min. The diluted HSQ
was processed by electron-beam lithography (EBL) at an acceleration
voltage of 20 kV with a dose of 800 μC cm−2 to define the dielectric
isolation layer, followed by developing in 25% tetramethylammonium
hydroxide solution for 60 s (Fig. 1a).
Single crystalline β-Ga2O3 substrates grown by the edge-defined
film-fed growth technique (Tamura Corp., effective electron carrier
density of ∼4 × 1017) were mechanically exfoliated into nanolayers
by using an adhesive tape. After a repetitive exfoliation process, a
β-Ga2O3 nanolayer was dry-transferred onto the p-diamond pre-
patterned with the HSQ dielectric layer as shown in Fig. 1b. The top
electrode metallization was defined with a standard EBL technique,
followed by electron-beam evaporation of Ti/Al/Ni/Au (20/40/20/
80 nm) (Fig. 1c) and low-vacuum thermal annealing at 470 °C under
Ar ambient at a pressure of 1 Torr.
The optical properties of the diamond substrate and the exfoliated
β-Ga2O3 nanolayer were evaluated by micro-Raman spectroscopy
under a back-scattering geometry at a wavelength of 532 nm using a
diode-pumped solid-state laser source (Omicron). The surface and
morphological properties were investigated by scanning electron
microscopy (SEM) (SU-70, Hitachi) and atomic force microscopy
(AFM) (Innova, Bruker). The temperature-dependent current-vol-
tage (I-V) characteristics were obtained with a semiconductor
parameter analyzer (Agilent 4155C). The optoelectronic properties
of the fabricated p-n heterojunction diode were characterized under
the illumination of a UV lamp (UVTECH) with the wavelengths of
365 nm (UV-A) and 254 nm (UV-C) in a low-vacuum chamber,
which allowed us to avoid the effects of ambient molecules such as
oxygen and ozone induced by the UV illumination.
Results and Discussion
The phonon modes of the exfoliated β-Ga2O3 nanolayer and the
diamond substrate were analyzed by micro-Raman spectroscopy
(Fig. 2a), which indicates that the crystallinity was maintained after
the device fabrication process. The three β-Ga2O3 phonon peaks at
100–200 cm–1 are ascribed to low-frequency vibration and translation
of tetrahedron–octahedron chains. The four phonon peaks ranging
from 300 to 500 cm−1 are attributed to the mid-frequency deforma-
tion of Ga2O6 octahedra. The peak at 750–800 cm−1 is assigned
to the high-frequency stretching and bending of GaO4 tetrahedra.
The Raman spectrum of the diamond shows a single phonon
peak at 1332 cm–1 with a full-width-at-half-maximum (FWHM) of
∼5.4 cm–1. The increased width of this signal compared to that of
pure diamond (FWHM ∼1.8 cm−1) is attributable to the relatively
high boron concentration.21 The optical microscopic and SEM images
are shown in Fig. 2b and in Supporting information (Fig. S1 is
available online at stacks.iop.org/JSS/9/045004/mmedia), respec-
tively, confirming the formation of an n-type β-Ga2O3 nanolayer
Figure 1. Schematics of the fabrication process of the mixed-dimensional diamond/β-Ga2O3 p-n heterojunction. (a) The HSQ dielectric layer was spin-coated on
the diamond and defined by an EBL technique. (b) A mechanically exfoliated β-Ga2O3 nanolayer was dry-transferred onto the p-diamond. (c) The top Ohmic
electrode to β-Ga2O3 was patterned by an EBL technique, followed by e-beam evaporation of Ti/Al/Ni/Au.
and p-diamond mixed-dimensional heterojunction. It seems that the
dark area (left) of the β-Ga2O3 nanolayer in Fig. 2b physically
contacted the p-diamond substrate. The difference in the color of the
β-Ga2O3 nanolayer implies that it bends around the HSQ dielectric
layer, and this is consistent with the AFM image in Fig. 2c. The van
der Waals interaction offers an abrupt and strain-free heterostructure
in various low-dimensional materials, allowing us to avoid the
dislocations induced by the lattice mismatch. The thickness and
root-mean-square roughness of the exfoliated Ga2O3 nanolayers were
200–300 nm and approximately 1 nm, respectively, which represent
the smoothness of the exfoliated Ga2O3 nanolayer. The height profile
of one of the exfoliated Ga2O3 nanolayers is shown in Fig. S2.
Figure 3a depicts the energy band diagram of the heterojunction
based on Anderson’s rule. The abrupt p-n heterojunction via a van der
Waals interaction was expected, where the electron affinity of p-
diamond and n-Ga2O3 are 0.5 and 4.0 eV, respectively.2,22 The
conduction band offset (ΔEC) and the valence band offset (ΔEV)
are estimated to be 3.5 and 2.9 eV, respectively. Since the dopant
concentrations of p-diamond and n-Ga2O3 are approximately 1019 and
4 × 1017, respectively, most of the depletion region is positioned
within the n-Ga2O3 nanolayer. Typical diode I-V characteristics were
obtained, as shown in Fig. 3b, where the rectification ratio was over
107 and the reverse leakage current was very low (<10−12 A) at room
temperature. The ideality factor (n) of the fabricated heterojunction
diode was calculated to be 6.8 at room temperature by using
the following equation: I = Is (exp (qV nkT ) - 1) , where Is is the
reverse saturation current, q is the electronic charge, V is the applied
voltage, n is the ideality factor, k is the Boltzman constant, and T is the
absolute temperature. The ideality factor of n-Ga2O3/p-diamond is
comparable to those of other β-Ga2O3 based heterostructures such as
n-Ga2O3/p-GaN (9.5–10 at room temperature)12 and n-Ga2O3/p-SiC
(>2.4 at room temperature).13 At elevated temperatures ranging from
298 to 423 K, the reverse leakage currents were around 10−11 A with
the rectifying behavior well maintained (Fig. 3c). At high tempera-
tures, a p-n diode is generally more robust than a Schottky diode since
the Schottky contact can react with the semiconductor. Also, the
reverse leakage current of a Schottky diode is usually higher than that
of a p-n diode under high reverse bias condition, which favors p-n
photodiodes over Schottky photodiodes because low dark current is
critical for a photodetector. The ideality factor (n) improved with
increasing temperature from 6.8 (at 298 K) to 3.5 (at 423 K), which is
in good agreement with the previous reports.12,13,23,24
The temperature dependence of the rectification ratio, turn-on
voltage, and reverse leakage currents are summarized in Figs. 3d and
3e. The rectification ratio decreased with increasing temperature
because of the increased reverse leakage current, although it
remained greater than 106 at 423 K. The diode turn-on voltage
also decreased with increasing temperature, which is consistent with
the electrical properties of typical p-n junction diodes. The diffusion
current across the space charge region will increase at elevated
temperatures, lowering the diode turn-on voltage as shown in
Fig. 3d. The activation energy was estimated to be ∼0.28 eV from
the Arrhenius plot of ln(current) vs 1/kT, which is in good agreement
with a previous report (Fig. 3e).25 The electrical hard breakdown of
the mixed-dimensional diamond/β-Ga2O3 p-n heterojunction was
observed at a reverse bias of 135 V (Fig. 3f), which is the highest
among β-Ga2O3 nanolayer-based diodes.26–28 This high breakdown
voltage is attributed to the high quality of both diamond and
 ECS Journal of Solid State Science and Technology, 2020 9 045004

Figure 2. (a) Raman spectra of the mechanically exfoliated β-Ga2O3 nanolayer (top) and the HPHT grown diamond (bottom). (b) Optical microscopy image and
(c) 3D AFM image of the fabricated diamond/β-Ga2O3 heterojunction. The scale bar is 10 μm.

Figure 3. (a) Band diagram of the diamond/β-Ga2O3 p-n heterojunction. (b) I–V characteristics of the diamond/β-Ga2O3 p-n heterojunction. The inset is on a
semi-logarithmic scale. (c) I–V characteristics of the diamond/β-Ga2O3 p-n heterojunction with increasing temperature. (d) Rectification ratio and turn-on
voltage with respect to temperature. (e) The Arrhenius plot of the current at a fixed voltage of −15 V. (f) The breakdown voltage (VBR) and an optical
microscope image of the diamond/β-Ga2O3 p-n heterojunction after electrical breakdown. The scale bar is 10 μm.

β-Ga2O3 crystals. The inset of Fig. 3f is the microscope image of the
device after the hard breakdown measurement, where the damage is
located at the spot of the bending. The microscopic image of the
device before the hard breakdown measurement is included in the
supporting information (Fig. S3). We believe that exfoliated
β-Ga2O3 nanolayers may be vulnerable when bent. Swinnich et al.
reported that the bending of a Ga2O3 nanolayer causes the formation
of defective states including micro-cracks.29 The optimization of the
device layout in a more nearly planar geometry could further
improve the hard breakdown voltage, pushing it close to the results
of thin-film β-Ga2O3 devices.
The photoresponse properties of the fabricated p-n heterojunction
diode were characterized under excitation at UV-A (365 nm) and UV-C
(254 nm) wavelengths, as shown in Fig. 4a. No photocurrent was
observed under exposure to the UV-A wavelength (365 nm). However,
a huge photocurrent of 4.0 × 10−9 A at a reverse bias of −15 V was
obtained under exposure to UV-C (254 nm) because electron-hole
pairs were generated by the band-to-band excitation, which explains the
solar-blindness of this diode (Fig. 4b). The excellent photoresponse
characteristics including high responsivity (12 A W−1), rejection ratio
(8500, R254nm/R365nm), and photo-to-dark-current ratio (PDCR, 3900)
were obtained, which are compared with the previously reported p-n
heterojunction photodiodes in Table SI (supplementary material).13,30–37
The time-dependent photoresponse to UV-C illumination (254 nm)
exhibited fast response and decay characteristics with excellent fidelity,
showing no persistent photoconductivity (PPC) (Fig. 4c). The rise time
 ECS Journal of Solid State Science and Technology, 2020 9 045004

Figure 4. (a) Schematic illustrating the mixed-dimensional diamond/β-Ga2O3 photodetector under illumination by the UV lamp. (b) I–V curves of the
diamond/β-Ga2O3 p-n heterojunction under dark and illuminated conditions. (c) Time-dependent photoresponse under 254 nm illumination at a fixed voltage of
−15 V; and (d) an enlarged view of the rise and decay times with fitted curves.

(which is defined as the time required to increase the photocurrent from
10% to 90% of its maximum current) under the UV-C exposure was
0.56 s. The decay time, needed to drop the photocurrent from 90% to
10% of its maximum current when the UV-C emission stopped, was
∼0.095 s. The response time was further analyzed as shown in Fig. 4d.
The rising edge showed bi-exponential growth behavior; thus, the curve
was fitted t using the following equation: I = I0 + A (1 - e- tr1 ) +
t
12 A/W, PDCR of 3900, rejection ratio of 8500 (R254nm/R365nm), no
PPC, and fast response and decay time constants of 0.56 and 0.095 s,
respectively. This p-n heterojunction based on mixed-dimensional
UWBG semiconductors allows us to utilize the full potentials of
their band-gap energies, opening a door to novel high-performance
(opto)electronic devices that can operate under harsh environments.

-
B (1 - e r2 ) , where I0 is the dark current, A and B are positive
t
38
Acknowledgments
constants, t is the time, and τr1 and τr2 are the risetime constants
The research at Korea University was supported by the National
estimated as 0.56 and 16 s, respectively. The decay edge was also
Research Foundation of Korea (2017M1A2A2087351), funded by
plotted by t using the following bi-exponential equation:
the Technology Development Program to Solve Climate Changes of
I = I0 + Ce- td1 + De- td 2 ,38 where C and D constants, and τd1 and
t

the National Research Foundation and the Korea Institute of Energy

τd2 are decay time constants estimated as 0.0951 and 3.5 s, respectively
(Fig. 4d). These time constants indicate fast rise and decay, and are
attributed to the nature of the p-n junction. The mixed-dimensional
heterostructure composed of the UWBG diamond and β-Ga2O3
semiconductors can pave a way for high performance nano-optoelec-
tronics and nano-electronics.
Conclusions
We demonstrated a mixed-dimensional UWBG p-n heterostruc-
ture by using a van der Waals interaction between a p-type diamond
substrate and an exfoliated n-type β-Ga2O3 nanolayer. Typical diode
I-V characteristics were observed under forward and reverse bias
conditions, exhibiting a high rectification ratio of >107 and a high
reverse hard breakdown voltage of 135 V. Robust electrical perfor-
mances including a high rectification ratio and low leakage currents
at elevated temperatures are attributed to the nature of a UWBG
semiconductor p-n junction. The optoelectronic properties of the
UWBG p-n heterojunction photodiode include a high responsivity of
Technology Evaluation and Planning (KETEP) (20172010104830).
The work at NUST MISiS was supported in part by the Ministry of
Education and Science of the Russian Federation in the framework
of the Increased Competitiveness Program of NUST (MISiS) (No.
K2-2017-068). Diamond sample preparation, characterization, me-
tallization and lithography in FSBI TISNCM were supported by RSF
(Project No. 18-72-00232).
ORCID
Sergey Tarelkin https://orcid.org/0000-0002-7278-3046
Alexander Polyakov https://orcid.org/0000-0001-6898-6126
Sergey Troschiev https://orcid.org/0000-0001-5505-6915
Jihyun Kim https://orcid.org/0000-0002-5634-8394
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