β-(AlxGa1−x)2O3/Ga2O3 (010) heterostructures

grown on β-Ga2O3 (010) substrates by

plasma-assisted molecular beam epitaxy
Cite as: J. Vac. Sci. Technol. A 33, 041508 (2015); https://doi.org/10.1116/1.4922340
Submitted: 11 April 2015 . Accepted: 28 May 2015 . Published Online: 10 June 2015

Stephen W. Kaun, Feng Wu, and James S. Speck

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© 2015 American Vacuum Society.

b-(AlxGa12x)2O3/Ga2O3 (010) heterostructures grown on b-Ga2O3 (010)
substrates by plasma-assisted molecular beam epitaxy
Stephen W. Kaun,a) Feng Wu, and James S. Speck
Materials Department, University of California, Santa Barbara, California 93106
(Received 11 April 2015; accepted 28 May 2015; published 10 June 2015)
By systematically changing growth parameters, the growth of b-(AlxGa1x)2O3/Ga2O3 (010)
heterostructures by plasma-assisted molecular beam epitaxy was optimized. Through variation of
the Al flux under O-rich conditions at 600  C, b-(AlxGa1x)2O3 (010) layers spanning 10% to
18% Al2O3 were grown directly on b-Ga2O3 (010) substrates. Nominal b-(AlxGa1x)2O3 (010)
compositions were determined through Al:Ga flux ratios. With x ¼ 0.18, the b-(AlxGa1x)2O3
(020) layer peak in a high-resolution x-ray diffraction (HRXRD) x-2h scan was barely discernible,
and Pendell€osung fringes were not visible. This indicated that the phase stability limit of Al2O3 in
b-Ga2O3 (010) at 600  C was less than 18%. The substrate temperature was then varied for a
series of b-(Al0.15Ga0.85)2O3 (010) layers, and the smoothest layer was grown at 650  C. The
phase stability limit of Al2O3 in b-Ga2O3 (010) appeared to increase with growth temperature, as
the b-(AlxGa1x)2O3 (020) layer peak with x ¼ 0.18 was easily distinguishable by HRXRD in a
sample grown at 650  C. Cross-sectional transmission electron microscopy (TEM) indicated that
b-(Al0.15Ga0.85)2O3 (010) layers (14.4% Al2O3 by energy dispersive x-ray spectroscopy) grown
at 650  C were homogeneous. b-(Al0.20Ga0.80)2O3 (010) layers, however, displayed a phase tran-
sition. TEM images of a b-(Al0.15Ga0.85)2O3/Ga2O3 (010) superlattice grown at 650  C showed
abrupt layer interfaces and high alloy homogeneity. V C 2015 American Vacuum Society.

[http://dx.doi.org/10.1116/1.4922340]

I. INTRODUCTION When grown on foreign substrates by molecular beam epi-

Si-based high-voltage electron devices have reached their
theoretical limits of performance—as a result, focus has
shifted toward devices based on wide-bandgap semiconduc-
tors.1 Recently, b-Ga2O3 has attracted attention for its large
bandgap of 4.8 eV,2,3 which leads to a high breakdown elec-
tric field, predicted to be 8 MV/cm.4 With a predicted maxi-
mum bulk electron mobility of 300 cm2/Vs, b-Ga2O3 yields
a Baliga figure of merit (BFOM)5 higher than that of 4H-SiC
and GaN.4 The BFOM is related to the minimum specific
on-resistance of a vertical electron device and promotes
b-Ga2O3 for low-loss, high-voltage switching applications.
High-breakdown Schottky diodes6 and field-effect transis-
tors4,7 have already been successfully fabricated on b-Ga2O3
epilayers. b-Ga2O3 also has potential as a substrate for GaN-
based light-emitting diodes and as a transparent conducting
oxide with favorable optical absorption characteristics.8,9
One major advantage of b-Ga2O3 epitaxy over GaN epi-
taxy in the realm of high-power electronics is the availability
of high-quality free-standing b-Ga2O3 substrates grown by
inexpensive melt methods. Bulk b-Ga2O3 crystals have been
produced through floating-zone,10,11 Czochralski,12,13 and
edge-defined film-fed growth.14 Conductive (Si-doped15 or
Sn-doped2) and semi-insulating (Fe-doped16) b-Ga2O3 sub-
strates with extremely low threading dislocation densities
(<105 cm2) are available for vertical and lateral electron
devices, respectively. Free-standing GaN substrates with
threading dislocation densities below 107 cm2 lack wide
availability and are commonly considered cost-prohibitive.
a)
Electronic mail: skaun@umail.ucsb.edu
taxy (MBE), the high threading dislocation density
(>109 cm2) of GaN-based high-electron-mobility transis-
tors (HEMTs) leads to vertical leakage and early degrada-
tion.17,18 Another advantage of b-Ga2O3 epitaxy over GaN
epitaxy is that oxygen, a common background impurity in
MBE, acts as a shallow donor19 in GaN, leading to uninten-
tionally doped (UID) GaN layers with relatively low resistiv-
ity. Highly resistive UID buffer layers are necessary for gate
control in lateral electron devices.
b-Ga2O3 exhibits the monoclinic b-gallia crystal structure
with the following lattice parameters: a ¼ 1.22 nm,
b ¼ 0.304 nm, c ¼ 0.580 nm, a ¼ c ¼ 90 , and b ¼ 103.8 .20
Initial b-Ga2O3 growth studies by MBE focused on the
strong-cleavage (100) plane.21 Although the weak ionic
bonds of the b-Ga2O3 (100) plane allow for high adatom dif-
fusivity, the decomposition rate of the (100) plane is rather
high. Homoepitaxial growth on b-Ga2O3 (100) is inhibited
by the formation of a highly volatile Ga2O suboxide through
the following reaction: Ga2O3 þ 4Ga ! 3Ga2O.22,23 Since
the homoepitaxial b-Ga2O3 (100) growth rate is very low,
lateral electron device structures with thick buffer layers are
not practical in this orientation. As such, research has
recently moved toward the noncleavage (010) orientation
where growth rates are reasonably high.24
The development of b-Ga2O3-based device structures
with alloyed b-(AlxGa1x)2O3 and b-(InxGa1x)2O3 layers is
still in its infancy. Thermally stable Al2O3 (8.7 eV
bandgap25) and In2O3 (2.9 eV bandgap26) have corundum27
and bixbyite28 crystal structures, respectively, so both are
expected to have limited solubility in b-Ga2O3.29–31 In an
equilibrium Al2O3-Ga2O3 phase diagram constructed by Hill

041508-1 J. Vac. Sci. Technol. A 33(4), Jul/Aug 2015 0734-2101/2015/33(4)/041508/9/$30.00 C 2015 American Vacuum Society
V 041508-1
041508-2 Kaun, Wu, and Speck: b-(AlxGa12x)2O3/Ga2O3 (010) heterostructures grown on b-Ga2O3 (010) substrates 041508-2

et al.,32 the solubility limit of Al2O3 in b-Ga2O3 was shown to

be 65% in the 850–1950  C temperature range. In the range
of temperatures commonly used by MBE (600–800  C), the
solubility limit of Al2O3 in b-Ga2O3 was drastically reduced
due to the formation of a AlGaO3 intermediate compound.
The b-(AlxGa1x)2O3/Ga2O3 heterostructure is of great
interest for its possible application to high-power HEMTs in
which the barrier layer (b-(AlxGa1x)2O3) is modulation-
doped. In an MBE growth study performed by Oshima
et al.,33 the solubility limit of Al2O3 in b-Ga2O3 (100) was
found to be 60% Al2O3 at 800  C, using x-ray photoelec-
tron spectroscopy to determine the composition. With a high
Al2O3 mole fraction in the barrier, the conduction band off-
set at the b-(AlxGa1x)2O3/Ga2O3 heterointerface would
allow the formation of a two-dimensional electron gas.
The growth study presented here provides the first investi-
gation of MBE growth parameters for (010)-oriented
b-(AlxGa1x)2O3/Ga2O3 heterostructures that can potentially
be used as HEMT structures. This study focuses on the sub-
strate temperature range (600–675  C) commonly used for
b-Ga2O3 (010) homoepitaxy. Phase stability limits of Al2O3
in b-Ga2O3 (010) are determined at 600 and 650  C, respec-
tively. Transmission electron microscopy (TEM) is then
used to determine b-(AlxGa1x)2O3 (010) alloy homogeneity
and b-(AlxGa1x)2O3/Ga2O3 (010) interfacial abruptness. FIG. 1. AFM height scans (1  1 lm2) of (a) a virgin b-Ga2O3 (010) sub-
strate, (b) a 100-nm-thick b-Ga2O3 (010) layer grown under O*-rich con-
II. EXPERIMENT ditions (AGa  AO* ¼ 0.2 nm/min) at 700  C (miscut direction inset), and
(c) a 100-nm-thick b-Ga2O3(010) layer grown under Ga-rich conditions
All layers were grown on 5  5 mm2 free-standing Fe- (AGa  AO* ¼ þ0.2 nm/min) at 700  C. The rms roughness values (hrms) of
doped b-Ga2O3 (010) substrates (Tamura). The b-Ga2O3 the AFM height scans are also included.
(010) substrates were vicinal with a 2.2 miscut approxi-
mately perpendicular to the h100i direction.34 Virgin sub- ranging from 600 to 675  C were used in this study. It was
strates had a root mean square (rms) surface roughness of also previously determined that O*-rich growth resulted in a
<0.2 nm [Fig. 1(a)] over an area of 1  1 lm2 with no visible favorable b-Ga2O3 (010) surface morphology, in comparison
step-terrace structure due to the large miscut angle. Before with Ga-rich growth. Ga-rich growth resulted in homoepitax-
entering the growth chamber, the substrates were solvent- ial b-Ga2O3 (010) layers with enhanced step-bunching and
cleaned, In-bonded to Si backing wafers, and outgassed in clusters at step edges [Fig. 1(c)]. For all growth series pre-
ultrahigh vacuum. Growth was performed in a Varian/Veeco sented here, the Ga BEP was fixed at 6.6  108 Torr to
620 MBE system equipped with conventional Ga and Al ensure that the metal flux (AGa,Al) was less than the active ox-
thermal effusion cells and a Veeco Uni-bulb oxygen rf- ygen flux (AO*).
plasma source. The substrate temperature was measured In the first Al flux series, 60 nm thick b-(AlxGa1x)2O3
with an optical pyrometer that was calibrated to the melting (010) layers were grown directly on b-Ga2O3 (010) sub-
point of Al (660  C). An oxygen foreline pressure of 60 Torr strates at 600  C. The Al BEP was varied from 0.7  108 to
and rf-plasma power of 200 W, corresponding to an active 1.4  108 Torr. b-(AlxGa1x)2O3 (010) layer compositions
oxygen (O*) beam equivalent pressure (BEP) of (nominal compositions of x ¼ 0.10, 0.12, 0.14, 0.15,
8.7  108 Torr, were maintained for all growths. The O* and 0.18) were estimated through Al:Ga flux ratios. In the
BEP was determined through growth rate calibrations. For substrate temperature series, 60 nm thick b-Ga2O3 (010)
Ga BEPs 8.7  108 Torr, the growth rate was stable at and b-(Al0.15Ga0.85)2O3 (010) layers (Al BEP of
3.2 nm/min. Before each growth, the b-Ga2O3 (010) sub- 1.2  108 Torr) were grown directly on b-Ga2O3 (010) sub-
strate was subjected to a oxygen plasma treatment for 30 min strates at 600, 625, 650, and 675  C. A second Al flux series
at 875  C to remove adsorbates from the surface. included 60 nm thick b-(AlxGa1x)2O3 (010) layers grown
Preliminary studies indicated a suitable substrate tempera- directly on b-Ga2O3 (010) substrates at 650  C. The Al BEP
ture range of 600–675  C for the homoepitaxial growth of in the second Al flux series was varied from 1.2  108 to
b-Ga2O3 (010). With a substrate temperature below 600  C, 1.6  108 Torr, resulting in b-(AlxGa1x)2O3 (010) layers
layer-by-layer growth occurred. With a substrate temperature with x ¼ 0.15, 0.18, and 0.20. b-(AlxGa1x)2O3/Ga2O3
above 675  C, step-bunching (formation of multisteps)35 was (010) heterostructures with 120 nm thick UID b-Ga2O3
apparent for relatively thin b-Ga2O3 (010) layers [Fig. 1(b)] (010) buffer layers were then grown at 650  C with Al BEPs
grown homoepitaxially. As such, substrate temperatures of 1.2  108 (x ¼ 0.15) and 1.6  108 Torr (x ¼ 0.20).

J. Vac. Sci. Technol. A, Vol. 33, No. 4, Jul/Aug 2015

041508-3 Kaun, Wu, and Speck: b-(AlxGa12x)2O3/Ga2O3 (010) heterostructures grown on b-Ga2O3 (010) substrates
An eight-period b-(Al0.15Ga0.85)2O3/Ga2O3 (010) super-
lattice was also grown at 650  C with 11.5 nm thick b-
(Al0.15Ga0.85)2O3 (010) layers (Al BEP of 1.2  108 Torr)
and 11 nm thick b-Ga2O3 (010) layers.
All structures were characterized with high-resolution x-ray
diffraction (HRXRD) using Cu Ka radiation in a PANalytical
X’pert Pro MRD system. An Asylum MFP3D atomic force mi-
croscopy (AFM) system was used to characterize the surface
morphology of the samples. In preparation for analysis by
TEM, specimens were extracted using an FEI Helios 600 Dual
Beam focused ion beam instrument. Scattering contrast TEM
images were taken with an FEI Tecnai G2 Sphera Microscope,
operated at 200 kV. High-angle annular dark-field scanning
TEM (HAADF-STEM) images were recorded with an FEI
Titan FEG Microscope, operated at 300 kV. Energy dispersive
x-ray spectroscopy (EDS) was used to assess the composition
of a b-(Al0.15Ga0.85)2O3 (010) layer (nominal composition
estimated by Al:Ga flux ratio).
III. RESULTS AND DISCUSSION
A. Al flux series at 600  C
60 nm thick b-(AlxGa1x)2O3 (010) layers were grown
directly on b-Ga2O3 (010) substrates to determine the phase
stability limit of Al2O3 in b-Ga2O3 (010) at 600  C.
Symmetric HRXRD x-2h scans around the b-Ga2O3 (020)
reflection for the Al flux series at 600  C are shown in Fig. 2.
As the Al2O3 mole fraction of the layer increased from 0.10
to 0.18, the separation between the b-(AlxGa1x)2O3 (020)
layer peak and b-Ga2O3 (020) substrate peak increased, corre-
sponding to a decrease in the (020) plane spacing. Assuming
coherently strained b-(AlxGa1x)2O3 layers, the reduction in
(020) plane spacing with increased Al2O3 mole fraction was
consistent with the reduction of unit cell volume shown in a
powder sintering study;31 thus, the compositions determined
by flux ratios were fairly accurate. With x ¼ 0.10, 0.12,
0.14, and 0.15, the b-(AlxGa1x)2O3 (020) layer peaks
were distinct with full widths at half maximum (FWHMs) of
FIG. 2. (Color online) Symmetric HRXRD x-2h scans around the b-Ga2O3 (020) reflection for the Al flux series at 600  C, which included 60 nm thick b-
(AlxGa1x)2O3 (010) layers grown on b-Ga2O3 (010) substrates.
JVST A - Vacuum, Surfaces, and Films
041508-3
540 arc sec, and Pendell€osung fringes indicated layer thick-
nesses of 55–58 nm. With x ¼ 0.18, the b-(AlxGa1x)2O3
(020) layer peak was barely distinguishable, and
Pendell€osung fringes were not visible. This indicated that the
b-(Al0.18Ga0.82)2O3 (010) layer was grown beyond the
phase stability limit of Al2O3 in b-Ga2O3 (010) at 600  C,
resulting in a polycrystalline layer.
AFM scans (1  1 lm2) of the b-(AlxGa1x)2O3 (010)
layers grown at 600  C are shown in Fig. 3. The root mean
square (rms) roughness of the b-(AlxGa1x)2O3 (010) layers
increased from 0.26 to 1.12 nm as the Al2O3 mole fraction
increased from 0.10 to 0.15. The depth and concentration
of surface depressions increased with increasing Al2O3 mole
fraction for samples grown below the Al2O3 phase stability
limit. This is likely the result of poor Al adatom surface dif-
fusivity at 600  C. Although the growth rate increased
slightly with increasing Al flux, kinetic restrictions intro-
duced by a higher growth rate would minimally impact the
surface morphology. With a substrate temperature of 600  C,
b-Ga2O3 (010) layers grown homoepitaxially at rates rang-
ing from 2.3 to 3.1 nm/min yielded similar surface character-
istics. The surface morphology of the b-(Al0.18Ga0.82)2O3
(010) layer, grown beyond the Al2O3 phase stability limit,
was different from the other samples in the Al flux series,
displaying an even distribution of islands. The surface
roughness (1.00 nm) of the b-(Al0.18Ga0.82)2O3 (010)
layer was also lower than that of the b-(Al0.15Ga0.85)2O3
(010) layer.
B. Substrate temperature series
The substrate temperature series included 60 nm thick
b-(Al0.15Ga0.85)2O3 (010) layers and homoepitaxial b-
Ga2O3 (010) layers grown at 600, 625, 650, and 675  C to
determine the effects of substrate temperature on surface
morphology. Symmetric HRXRD x-2h scans around the b-
Ga2O3 (020) reflection for the b-(Al0.15Ga0.85)2O3 (010)
layers in the substrate temperature series are shown in Fig. 4.
041508-4 Kaun, Wu, and Speck: b-(AlxGa12x)2O3/Ga2O3 (010) heterostructures grown on b-Ga2O3 (010) substrates 041508-4

FIG. 3. AFM height scans (1  1 lm2) of b-(AlxGa1x)2O3 (010) layers grown at 600  C with x ¼ 0.10, x ¼ 0.12, x ¼ 0.14, x ¼ 0.15, and x ¼ 0.18.
The height scale is 10 nm. The rms roughness values (hrms) of the AFM height scans are also included.

These x-2h scans showed distinct b-(Al0.15Ga0.85)2O3 Ga2O3 (010) layers. In a study performed by Sasaki et al.,24
(020) layer peaks with consistent FWHMs of 540 arc sec the homoepitaxial growth rate of b-Ga2O3 was reduced by
that were separated from the b-Ga2O3(020) substrate peaks 30% on the (001) plane, in comparison with growth on the
by 0.84 –0.87 . The Pendell€osung fringes in Fig. 4 indicated (010) plane. The homoepitaxial growth rate of b-Ga2O3
b-(Al0.15Ga0.85)2O3 (010) layer thicknesses of 55–59 nm. (001) is presumably reduced by the formation of the Ga2O
Due to a rigid body displacement at the growth interface,36
the homoepitaxial b-Ga2O3 (010) layers also displayed
Pendell€osung fringes in HRXRD x-2h scans, indicating b-
Ga2O3 (010) layer thicknesses of 58–60 nm.
AFM scans (1  1 lm2) of the substrate temperature se-
ries are shown in Fig. 5. As the substrate temperature
increased from 600 to 675  C, the rms roughness of the
homoepitaxial b-Ga2O3 (010) layers increased from 0.60 to
1.12 nm. Step edges were not evident on the surface of the
homoepitaxial b-Ga2O3 (010) layer grown at 600  C, but
could be seen when the substrate temperature increased to
625  C. With substrate temperatures above 625  C, step-
bunching became more pronounced in the homoepitaxial b-

FIG. 4. (Color online) Symmetric HRXRD x-2h scans around the b-Ga2O3 FIG. 5. (Color online) AFM height scans (1  1 lm2) of 60 nm thick b-
(020) reflection for the substrate temperature series, which included 60 nm Ga2O3 (010) and b-(Al0.15Ga0.85)2O3 (010) layers grown with substrate
thick b-(Al0.15Ga0.85)2O3 (010) layers grown on b-Ga2O3 (010) substrates temperatures of 600, 625, 650, and 675  C. The height scale is 10 nm. The
at 600, 625, 650, and 675  C. rms roughness values (hrms) of the AFM height scans are also included.

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041508-5 Kaun, Wu, and Speck: b-(AlxGa12x)2O3/Ga2O3 (010) heterostructures grown on b-Ga2O3 (010) substrates 041508-5

suboxide. Since the miscut exposed steps oriented approxi- layers grown at 700  C would likely provide a different surface
mately in the h100i direction ((001) plane steps), step- morphology than that shown in Fig. 1(c).
bunching was likely caused by Ga2O suboxide formation at
the step edges. C. Al flux series at 650  C
As shown in Fig. 5, the presence of Al2O3 suppressed The smoothest b-(Al0.15Ga0.85)2O3 (010) layer in the sub-
step-bunching, as step edges were not visible on the strate temperature series was grown at 650  C, which was
b-(Al0.15Ga0.85)2O3 (010) layers grown with substrate tem- determined to be the optimal b-(AlxGa1x)2O3(010) growth
peratures ranging from 600 to 675  C. Whereas the rms rough- temperature. The second Al flux series was grown at 650  C
ness of the homoepitaxial b-Ga2O3 (010) layers increased with to assess the Al2O3 phase stability limit at the optimal
increasing substrate temperature, the rms roughness of the b-(AlxGa1x)2O3 (010) growth temperature. b-(AlxGa1x)2O3
b-(Al0.15Ga0.85)2O3 (010) layers decreased from 1.12 to (010) layers were grown at 650  C with x ¼ 0.15, 0.18, and
0.50 nm as the substrate temperature increased from 600 to 0.20. Symmetric HRXRD x-2h scans (Fig. 6) of the Al flux
650  C. The increased thermal energy presumably aided series grown at 650  C showed distinct b-(AlxGa1x)2O3 (020)
the surface diffusion of Al adatoms. With growth at 675  C, the layer peaks for x ¼ 0.15 and 0.18. With x ¼ 0.18, how-
b-(Al0.15Ga0.85)2O3 (010) layer had an rms roughness slightly ever, Pendell€osung fringes around the b-(AlxGa1x)2O3 (020)
higher than the b-(Al0.15Ga0.85)2O3 (010) layer grown at layer peak were poorly defined. The phase stability limit of
650  C and showed similar surface features to those of the
homoepitaxial b-Ga2O3 (010) layer grown at 625  C. While the
trend of enhanced step-bunching with increased substrate tem-
perature was clear for the homoepitaxial b-Ga2O3 (010) layers,
a trend in surface features with substrate temperature was not
easily identified for the b-(Al0.15Ga0.85)2O3 (010) layers. The
surface features of the b-(Al0.15Ga0.85)2O3 (010) layers may
have been largely influenced by the surface features of the
b-Ga2O3 (010) substrate after the oxygen plasma treatment.
The metal-rich regime should be explored for b-
(Al0.15Ga0.85)2O3 (010) layers grown directly on b-Ga2O3
(010). It was assumed that excess Ga would lead to surface clus-
ters oriented along bunched step edges, which was the result of
Ga-rich b-Ga2O3 (010) homoepitaxy at 700  C [Fig. 1(c)].
Assuming that the inclusion of Al2O3 suppresses step-bunching
during metal-growth, metal-rich b-(Al0.15Ga0.85)2O3 (010)

FIG. 7. AFM height scans (1  1 lm2) of 60 nm thick b-(AlxGa1x)2O3

FIG. 6. (Color online) Symmetric HRXRD x-2h scans around the b-Ga2O3 (010) layers grown at 650  C with x ¼ 0.15, x ¼ 0.18, and x ¼ 0.20.
(020) reflection for the Al flux series at 650  C, which included 60 nm The height scale is 10 nm. The rms roughness values (hrms) of the AFM
thick b-(AlxGa1x)2O3 (010) layers grown on b-Ga2O3 (010) substrates. height scans are also included.

JVST A - Vacuum, Surfaces, and Films

041508-6 Kaun, Wu, and Speck: b-(AlxGa12x)2O3/Ga2O3 (010) heterostructures grown on b-Ga2O3 (010) substrates 041508-6

FIG. 8. (Color online) Cross-sectional HAADF-STEM (a) and bright-field TEM (b) images taken from the [001] zone axis projection of a 60 nm thick b-
(Al0.15Ga0.85)2O3 (010) layer grown at 650  C. The diffraction pattern of the b-(Al0.15Ga0.85)2O3 (010) layer is overlaid on the bright-field TEM image.
Cross-sectional HAADF-STEM (c) and bright-field TEM (d) images (diffraction pattern overlaid) taken from the [001] zone axis projection of a 60 nm thick
b-(Al0.20Ga0.80)2O3 (010) layer grown at 650  C are also shown. With an Al2O3 mole fraction beyond the phase stability limit, the b-(Al0.20Ga0.80)2O3
(010) layer shows faceting upon growth initiation and the appearance of a second phase.

Al2O3 in b-Ga2O3 (010) during growth at 650  C appeared to
be near 18%. Seeing that the b-(Al0.18Ga0.82)2O3 (020) layer
peak was barely distinguishable through growth at 600  C,
the phase stability limit of Al2O3 in b-Ga2O3 (010) appeared
to increase with increasing substrate temperature. The
b-(Al0.20Ga0.80)2O3 (010) layer was grown beyond the phase
stability limit of Al2O3 in b-Ga2O3 (010), as evidenced by the
weak b-(Al0.20Ga0.80)2O3 (020) layer peak and lack of
Pendell€osung fringes.
AFM scans (1  1 lm2), shown in Fig. 7, of the Al flux se-
ries at 650  C yielded a similar roughness trend to that of the
Al flux series at 600  C. The highest rms roughness (1.24 nm)

FIG. 9. (Color online) Symmetric HRXRD x-2h scans around the b-Ga2O3 (020) reflection for b-(AlxGa1x)2O3/Ga2O3 (010) heterostructures with 120 nm
thick UID b-Ga2O3 (010) buffers. AFM height scans (1  1 lm2) and 1D height profiles (inset) of b-(Al0.20Ga0.80)2O3/Ga2O3 (010) and b-
(Al0.15Ga0.85)2O3/Ga2O3 (010) heterostructures are also included. The height scale is 10 nm. The rms roughness values (hrms) of the AFM height scans are
noted.

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041508-7 Kaun, Wu, and Speck: b-(AlxGa12x)2O3/Ga2O3 (010) heterostructures grown on b-Ga2O3 (010) substrates 041508-7

in the Al flux series at 650  C was measured on the
b-(Al0.18Ga0.82)2O3 (010) layer, which was grown close to
the Al2O3 phase stability limit. The rms roughness then
decreased to 0.60 nm in the b-(Al0.20Ga0.80)2O3 (010) layer,
which was grown beyond the Al2O3 phase stability limit at
650  C. A similar reduction in rms roughness and islanded
morphology was seen for the b-(Al0.18Ga0.82)2O3 (010)
layer grown beyond the phase stability limit in the first Al flux
series at 600  C.
Cross-sectional HAADF-STEM was performed in the
[001] zone axis projection of the b-(Al0.15Ga0.85)2O3 (010)
layer from the Al flux series grown at 650  C. Since HAADF-
STEM intensity depends on the atomic number of the ele-
ments present, darker contrast (lower intensity) indicates a
higher Al2O3 mole fraction. The b-(Al0.15Ga0.85)2O3 (010)
layer appeared to be homogeneous by HAADF-STEM
[Fig. 8(a)], verifying that an Al2O3 mole fraction of 0.15 is
below the phase stability limit at 650  C. EDS performed on
the b-(Al0.15Ga0.85)2O3 (010) layer yielded 14.4% Al2O3,
confirming the accuracy of the compositions determined
through flux ratios. Bright-field TEM shows a contrast trend
opposite that of HAADF-STEM, so lighter contrast in bright-
field TEM indicates a higher Al2O3 mole fraction. With
bright-field TEM, the b-(Al0.15Ga0.85)2O3 (010) layer
[Fig. 8(b)] again appeared to be homogeneous. The vertical
contrast grading in Fig. 8(b) was the result of Pendell€osung
fringing. The HAADF-STEM image [Fig. 8(c)] of the
b-(Al0.20Ga0.80)2O3 (010) layer showed lateral and
vertical inhomogeneity. Upon growth initialization, the
b-(Al0.20Ga0.80)2O3 (010) layer became faceted, and a
new phase appeared. In the bright-field TEM image [Fig.
8(d)] of the b-(Al0.20Ga0.80)2O3 (010) layer, the layer was
clearly polycrystalline, confirming that 20% Al2O3 is
beyond the phase stability limit at 650  C.
that formed between the bunched steps were 2–6 nm deep, as
shown in the inset of Fig. 9. Step-bunching in AlGaN/GaN
and InAlN/GaN heterostructures grown on vicinal substrates
has been shown to significantly reduce the electron mobility
perpendicular to the bunched step edges.37 Minimizing these
height fluctuations will be a point of emphasis in the growth
of b-(AlxGa1x)2O3/Ga2O3 (010) HEMT structures. It is
likely that UID b-Ga2O3 (010) buffer layers will need to be
grown at lower temperatures (600  C) than b-
(AlxGa1x)2O3 (010) barriers (650  C) to reduce the sur-
face roughness. It may also be necessary to include a b-
(AlxGa1x)2O3 (010) layer in the buffer. The addition of a b-
(AlxGa1x)2O3 (010) buffer layer would enhance the separa-
tion between the device channel and growth interface with-
out increasing the surface roughness, as the alloy seems to
suppress step-bunching. The b-(AlxGa1x)2O3 (010) buffer
layer would also act as a natural back barrier.
The surface of the b-(Al0.20Ga0.80)2O3/Ga2O3 (010) het-
erostructure (polycrystalline barrier) had an rms roughness of
0.68 nm, which was much lower than the rms roughness
(1.72 nm) of the b-(Al0.15Ga0.85)2O3/Ga2O3 (010)

D. b-(AlxGa12x)2O3/Ga2O3(010) heterostructures with

UID b-Ga2O3(010) buffer layers
Adding an UID b-Ga2O3 (010) buffer layer between
the b-(AlxGa1x)2O3 (010) barrier and Fe-doped b-Ga2O3
(010) substrate will be essential for the realization of b-
(AlxGa1x)2O3/Ga2O3 (010) HEMTs. b-(AlxGa1x)2O3/
Ga2O3 (010) heterostructures with 120 nm thick b-Ga2O3
(010) buffer layers were grown at 650  C to determine the
effects of the buffer layer on the surface morphology. The b-
(AlxGa1x)2O3 (010) barrier thickness was maintained at
60 nm for comparison with the aforementioned growth se-
ries. As shown in Fig. 9, the b-(AlxGa1x)2O3 (020) barrier
peak in HRXRD x-2h scans was distinct with x ¼ 0.15,
but weak with x ¼ 0.20, as described previously. In the
HRXRD scan of the b-(Al0.15Ga0.85)2O3/Ga2O3 (010) het-
erostructure, fringes that resulted from uniform rigid body
displacement at the growth interface were seen around the b-
Ga2O3 (020) peak. FIG. 10. (Color online) (a) Layer schematic of an eight-period b-
The surface morphology [Fig. 9] of the b- (Al0.15Ga0.85)2 O3/Ga2O3 (010) superlattice grown at 650  C. (b)
Symmetric HRXRD x-2h scan around the b-Ga2O3 (020) reflection for the
(Al0.15Ga0.85)2O3/Ga2O3 (010) heterostructure was domi-
b-(Al0.15Ga0.85)2O3/Ga2O3 (010) superlattice. (c) AFM height scan (1 
nated by step-bunching that evolved during growth of the 1 lm2) of the superlattice and 1D height profile. The height scale is 10 nm.
120 nm thick UID b-Ga2O3(010) buffer layer. The grooves The rms roughness (hrms) of the AFM height scan is noted.

JVST A - Vacuum, Surfaces, and Films

041508-8 Kaun, Wu, and Speck: b-(AlxGa12x)2O3/Ga2O3 (010) heterostructures grown on b-Ga2O3 (010) substrates
FIG. 11. Cross-sectional HAADF-STEM image taken from the [201] zone axis projection of an eight-period b-(Al0.15Ga0.85)2O3/Ga2O3 (010) superlattice
grown at 650  C.
heterostructure. The polycrystalline barrier appeared to fill in
the grooves that evolved during growth of the UID b-Ga2O3
(010) buffer layer. The b-(Al0.20Ga0.80)2O3/Ga2O3 (010)
heterostructure had grooves that were only 1–2 nm in depth
and exhibited a islanded surface morphology similar to the b-
(Al0.20Ga0.80)2O3 (010) layer in the Al flux series at
650  C.
E. b-(Al0.15Ga0.85)2O3/Ga2O3(010) superlattice
To assess the effects of step-bunching on alloy homoge-
neity, an eight-period b-(Al0.15Ga0.85)2O3/Ga2O3 (010)
superlattice [Fig. 10(a)] with 11.5 nm thick b-
(Al0.15Ga0.85)2O3 (010) layers and 11 nm thick b-Ga2O3
(010) layers was grown at 650  C. The HRXRD x-2h scan
[Fig. 10(b)] of the superlattice around the b-Ga2O3 (020)
peak showed sharp layer peaks and thickness fringes, indi-
cating abrupt interfaces and intended periodicity. The AFM
image [Fig. 10(c)] of the superlattice indicated a surface
dominated by bunched steps, much like that of the b-
(Al0.15Ga0.85)2O3/Ga2O3 (010) heterostructure with the
120 nm thick UID b-Ga2O3 (010) buffer layer. However,
the rms roughness (1.40 nm) and average groove depth
(2 nm) of the superlattice were lower than those of b-
(Al0.15Ga0.85)2O3/Ga2O3 (010) heterostructure with the
UID b-Ga2O3(010) buffer layer, despite having the same
total thickness (180 nm). The total b-(Al0.15Ga0.85)2O3
(010) thickness was 92 nm in the superlattice, whereas the
total b-(Al0.15Ga0.85)2O3 (010) thickness was 60 nm in the
heterostructure with the UID buffer layer. b-
J. Vac. Sci. Technol. A, Vol. 33, No. 4, Jul/Aug 2015
041508-8
(Al0.15Ga0.85)2O3 (010) comprised a greater percentage of
the superlattice than the heterostructure with the UID buffer
layer. The lower roughness and groove depth of the superlat-
tice followed the trend of b-(Al0.15Ga0.85)2O3 (010)
growth not contributing to step-bunching.
As shown in the HAADF-STEM image (Fig. 11) of the
b-(Al0.15Ga0.85)2O3/Ga2O3 (010) superlattice, the b-
(Al0.15Ga0.85)2O3 (010) layers displayed high alloy ho-
mogeneity, indicated by relatively uniform lateral contrast.
The initial layers of the superlattice were very flat with uni-
form alloy distribution. At the end of the third period from
the growth interface, dips began to form at layer interfaces,
designating the onset of step-bunching. In the upper magni-
fied portion of the HAADF-STEM image, the contrast
appears slightly darker at the dip in the interface, which
could possibly indicate a higher Al2O3 mole fraction. This
may also be an artifact of specimen thickness variation, as
the b-Ga2O3 (010) also appears darker in this region.
Regardless, the interface abruptness and homogeneous
alloy distribution shown in Fig. 11 indicate that b-
(Al0.15Ga0.85)2O3/Ga2O3 (010) heterostructures can be
used for electron devices.
IV. CONCLUSIONS
Through Al flux variation, the phase stability limit of
Al2O3 in b-Ga2O3 (010) at 600  C was determined to be
15%. Through substrate temperature variation, the optimal
growth temperature of b-(Al0.15Ga0.85)2O3 (010) was
041508-9 Kaun, Wu, and Speck: b-(AlxGa12x)2O3/Ga2O3 (010) heterostructures grown on b-Ga2O3 (010) substrates
determined to be 650  C since this temperature resulted in 8
the smoothest layer. Unlike homoepitaxial b-Ga2O3 (010), 9
b-(Al0.15Ga0.85)2O3 (010) did not display step-bunching 10
for a layer thickness of 60 nm through the range of sub-
11
strate temperatures (600–675  C) studied. With a substrate
temperature of 650  C, the phase stability limit of Al2O3 in 12
b-Ga2O3 (010) appeared to expand to 18%. A b-
13
(Al0.15Ga0.85)2O3/Ga2O3 (010) heterostructure with a UID 14
b-Ga2O3(010) buffer layer and an eight-period b-
(Al0.15Ga0.85)2O3/Ga2O3 (010) superlattice were success- 15
fully grown at 650  C. HAADF-STEM images of the b-
16
(Al0.15Ga0.85)2O3/Ga2O3 (010) superlattice indicated ho-
mogeneous alloy distribution and abrupt layer interfaces. 17
The phase stability limits of Al2O3 at 600 and 650  C by
MBE were similar to the Al2O3 solubility limits in the equi- 18
librium Al2O3-Ga2O3 phase diagram developed by Hill
19
et al.32 Presumably, growth of b-(AlxGa1x)2O3 (010) at 20
substrate temperatures near 800  C will drastically enhance
21
the Al2O3 phase stability limit. To accomplish high Al2O3
content growth at high temperature, the O* flux must be 22
improved through rf plasma source modification. With a
high O* flux, the b-(AlxGa1x)2O3 (010) growth parameter 23
24
space will expand, and high-quality high-rate growth can be
accomplished. 25
26
ACKNOWLEDGMENTS
This work was supported by the MRSEC Program of the 27
U.S. National Science Foundation under Award No. DMR-
28
1121053. The authors also thank John English and Kurt
29
Olsson for help with MBE system maintenance.
30
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