Article

Journal of
Copyright © 2016 American Scientific Publishers
Nanoscience and Nanotechnology
All rights reserved Vol. 16, 11575–11579, 2016
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Improvement of Epitaxial GaN Films Grown on Patterned

Sapphire Substrate by Growth Mode Control
Dae-Sik Kim1 , Chang-Min Lee1 , Woo Seop Jeong1 , Seung Hee Cho1 ,
Junggeun Jhin2 , and Dongjin Byun1
∗
1
Department of Materials Science and Engineering, Korea University, Seoul 02841, Korea
2
Quality Planning Team, Quality Management Division, LG Innotek, Seoul 04637, Korea

Epitaxial GaN films were grown via metal-organic chemical vapor deposition (MO-CVD) on a cone-
shaped patterned sapphire substrate (PSS). A 25 nm thick AlN was deposited by ex-situ sputtering
as a buffer layer. The GaN films were grown under various conditions by controlling the substrate
temperature (1020–1100  C) and working pressure (85–300 Torr). GaN films grown on PSS via
the conventional two-step growth mode consisting of vertical (three-dimensional; 3D) growth and
horizontal (two-dimensional; 2D) growth contained poly-grains on top of the cone-shaped pattern.
The growth of multi-directional poly-grains on top of the cone-shaped pattern generated numerous
defects even though the GaN films were grown by the epitaxial lateral overgrowth (ELO) process.
In this paper, we introduce an effective method to control the growth mode of GaN on PSS during the
ELO process. The GaNby
Delivered films grown to:
Ingenta on PSS
StateviaUniversity
the optimized growth
of New mode
York control showed improve-
at Binghamton
ment of crystal qualityIP:
and95.181.217.73 On: Thu,
surface roughness. 18 May
The surface 2017 06:39:18
morphology and roughness of the GaN
Copyright: American
films were investigated by field-emission scanning Scientific Publishers(FE-SEM) and atomic force
electron microscopy
microscopy (AFM) in non-contact mode, respectively. The crystal quality of the GaN films was eval-
uated by
–2 high-resolution X-ray diffraction (HR-XRD) and the cathodoluminescence (CL) was
measured in the 300–800 nm wavelength range to confirm the distribution of threading dislocations.
Keywords: Gallium Nitride, Thin Film, Patterned Sapphire Substrate, Epitaxial Lateral
Overgrowth, Metal-Organic Chemical Vapor Deposition.

1. INTRODUCTION issues, the technology of a micro- or nano-scale patterned

Gallium nitride (GaN)-based materials are key materials
for optoelectronic devices such as short-wavelength light
emitting diodes (LEDs)1
2 and laser diodes (LDs).3
4 High
quality GaN epitaxial layer on sapphire substrates have
attracted a great deal of attention for improving the effi-
ciency of these devices. In general, the external quantum
efficiency of LEDs comprises the internal quantum effi-
ciency (IQE) and light extraction efficiency (LEE). The
IQE is seriously affected by the threading dislocation (TD)
density and misfit because of the large thermal expan-
sion coefficient and lattice mismatch between the GaN
epitaxial layer and sapphire substrate.5–7 The LEE is lim-
ited by total internal reflection (TIR), which is due to the
large difference of refractive index between the devices
and surrounding air. In order to resolve the IQE and LEE
∗
Author to whom correspondence should be addressed.
sapphire substrate (PSS) has been widely reported.8 The
PSS can effectively reduce the TD density and misfit
by epitaxial lateral overgrowth (ELO) and improve the
LEE by extending the critical angle of the escape cone.9
However, epitaxial GaN films grown on PSS through the
conventional two-step growth mode, well known, consist-
ing of vertical (3D) growth and horizontal (2D) growth
include poly-grains on the top of the cone-shaped pat-
tern. The poly-grains grown in different crystal directions
are a cause of the TD and non-radiative centers.10 In this
paper, we introduce an effective growth mode for depo-
sition of epitaxial GaN films on PSS without growth of
the poly-grains on the top of the cone-shaped pattern
via metal-organic chemical vapor deposition. The epitax-
ial GaN films grown via the optimized growth mode show
improvement of crystal quality and surface roughness rel-
ative to the epitaxial GaN films grown by the conventional
two-step growth mode.

J. Nanosci. Nanotechnol. 2016, Vol. 16, No. 11 1533-4880/2016/16/11575/005 doi:10.1166/jnn.2016.13554 11575

Improvement of Epitaxial GaN Films Grown on Patterned Sapphire Substrate by Growth Mode Control
2. EXPERIMENTAL DETAILS
Epitaxial GaN films were grown on cone-shaped PSS
(4.0 m diameter and 1.6 m height) by using a home-
made MOCVD system consisting of a horizontal quartz
glass and silicon carbide susceptor. AlN buffer layers
(25 nm thickness) were deposited on PSS by ex-situ
sputtering to relax the stress between the epitaxial GaN
films and PSS. Trimethylgallium (TMGa, Ga(CH3 3 ) and
ammonia (NH3 , 99.9999% purity) were used as the pre-
cursors for gallium and nitrogen, respectively. The TMGa
precursor was allowed to flow directly into a home-
made horizontal reactor by using hydrogen (H2 , 99.9999%
purity) carrier gas. The TMGa precursor was maintained
at −10  C to control the excess vapor pressure. In order
to maintain the group III/V ratio, the flow rates of TMGa
and NH3 were controlled at 8.0 sccm and 2.0 slm, respec-
tively. Growth of the GaN film was carried out in three
steps as shown the process time chart for GaN growth in
Figure 1. The 1st step of the growth process was the ver-
tical (3D) growth mode performed at low temperature and
high pressure without generating poly-grains on the top
of the cone-shaped pattern. The 2nd step of the growth
process involved simultaneous vertical (3D) and horizon-
tal (2D) growth mode. The 3rd step of the growth process
involved the horizontal (2D) growth mode at high tem-
perature and low pressure, known as the ELO process for
GaN. Epitaxial GaN films of the by
Delivered three types to:
Ingenta of State
samples
University of New YorkAND
on PSS were produced by combination of the respective
IP: 95.181.217.73 On: Thu,The
steps, as shown in Table I. The A,Copyright: B, and C American
samples Scientific
were subjected to the same conditions of the most com-
monly used 2-step growth mode, consisting of the 1st step
(1020  C, 300 Torr, 10 min.) for vertical (3D) growth
Figure 1. Process time chart for MO-CVD system used for deposition
of epitaxial GaN films on PSS.
11576
Kim et al.
Table I. Conditions for growth of epitaxial GaN films on PSS via three-
step mode.
Growth condition 1st step 2nd step 3rd step
I (sample A) 1020  C 1100  C
85 Torr
30 min. + 60 min.
II (sample B) 300 Torr 1050  C 1100  C
85 Torr 85 Torr
30 min. 60 min.
III (Sample C) 10 min. 1020  C 1100  C
85 Torr 85 Torr
30 min. 60 min.
and the 3rd step (1100  C, 85 Torr, 60 min.) for horizon-
tal (2D) growth. On the other hand, the additional 2nd
step was carried out under each condition (1020–1100  C,
85 Torr, 30 min.). The surface morphology and rough-
ness of GaN films were investigated by field-emission
scanning electron microscopy (FE-SEM) and atomic force
microscopy (AFM) in non-contact mode, respectively.
The crystal quality of the GaN films was evaluated by
–2 high resolution X-ray diffraction (HR-XRD) and
cathodoluminescence (CL) was acquired in the wavelength
range of 300–800 nm to confirm the distribution of the
TD centers.
3. RESULTS
DISCUSSION
at Binghamton
18 May 2017images
FE-SEM 06:39:18
presented in Figures 2(a–f) clearly
reveal thePublishers
morphologies of the epitaxial GaN films grown
on PSS under different conditions (i.e., growth conditions
I, II, and III). As shown in Figures 2(a–c), the epitaxial
GaN films were successfully grown without any v-defects
and hillock on the surface. Despite the different growth
conditions, all samples had a smooth and mirror-like flat
surface. Sample A (4.85 m thick) and the sample B
(4.40 m thick), shown in Figures 2(d and e), contained
poly-grains on the top of the cone-shaped pattern, whereas
for sample C (4.50 m thick), the cone-shaped pattern was
confirmed to have a very clean surface.
Figures 2(g–i) show schematic diagrams of the cross-
sectional view. Generally, GaN films are grown in the
shape of a trapezoid under relatively low temperature and
high pressure conditions, such as used for the 1st step.
Since the N -polarity surface region 112̄2 is stabilized
under this condition (i.e., condition I), the growth rate of
the lateral direction decreases, and vertical (3D) growth
of the [0001] direction becomes dominant.11
12 However,
poly-grains were grown over the entire surface of the cone-
shaped pattern for sample A, as shown in Figure 2(g). The
slop area of the cone-shaped pattern is similar to the r-like
plane of the crystal structure.13
The surface energy of the c-plane (7.4 J · m−2 ) is higher
than that of the r-plane (5.9 J · m−2 ).14 This means that
poly-grains, supplied with enough energy, were grown dur-
ing the 2nd step and 3rd step of the process. In the case
J. Nanosci. Nanotechnol. 16, 11575–11579, 2016
Kim et al. Improvement of Epitaxial GaN Films Grown on Patterned Sapphire Substrate by Growth Mode Control

Delivered by Ingenta to: State University of New York at Binghamton

IP: 95.181.217.73 On: Thu, 18 May 2017 06:39:18
Figure 2. FE-SEM images (a)–(c) top view, (d)–(f) cross sectional view, and (g)–(i) schematic diagram of the epitaxial GaN films on PSS formed
Copyright: American Scientific Publishers III. Condition I: 1020  C,
under different growth condition (a), (d), and (g): condition I, (b), (e), and (h): condition II, (c), (f), and (i): condition
300 Torr, 10 min. +1100 C, 85 Torr, 30 min. +1100 C, 85 Torr, 60 min. Condition II: 1020 C, 300 Torr, 10 min. +1050  C, 85 Torr, 30 min.
  

+1100  C, 85 Torr, 60 min. Condition III: 1020  C, 300 Torr, 10 min. +1020  C, 85 Torr, 30 min. +1100  C, 85 Torr, 60 min.

of sample B (Fig. 2(h)), the energy supplied was relatively
lower than that supplied to sample A during the 2nd step
process. Therefore, the poly-grains were grown on the c-
like plane of the cone during the 3rd step process. Sam-
ple C (Fig. 2(i)) shows the optimized growth mode of
the epitaxial GaN films on PSS. The 2nd step of con-
dition III is necessary for the merging process without
generation of poly-grains on the cone-shaped pattern. The
N-polarity surface region 112̄2 becomes relatively unsta-
ble under high temperature and low pressure conditions,
such as those used for the 3rd step. Therefore, the growth
rate of the lateral direction increased and horizontal (2D)
growth becomes dominant.11
12 Figures 3(a–c) show the
300 nm to 800 nm wavelength panchromatic CL images of

Figure 3. Panchromatic (300 nm–800 nm; CL) images of the epitaxial GaN films of (a) sample A, (b) sample B, and (c) sample C grown on PSS
under different conditions: (a) condition I, (b) condition II, and (c) condition III.

J. Nanosci. Nanotechnol. 16, 11575–11579, 2016 11577

Improvement of Epitaxial GaN Films Grown on Patterned Sapphire Substrate by Growth Mode Control Kim et al.

Figure 4. AFM images of the epitaxial GaN films of (a) sample A, RMS: 0.547 nm, (b) sample B, RMS: 0.469 nm, and (c) sample C, RMS:
0.169 nm grown on PSS under different conditions: (a) condition I, (b) condition II, and (c) condition III.

the sample A, B, and C, respectively. The TDs of the three
sample types are divided into edge, screw and mixed dislo-
cations. The screw type dislocations lead to non-radiative
centers,15 thus they are represented by dark spots in the
CL images.16
17 As shown Figure 3(a), the dark spots are
localized around the cone-shaped pattern. As the number
of poly-grains formed on the cone-shaped area increases,
the incidence of the TD on the surface increases. The
panchromatic image of sample C in Figure 3(c) shows the
002
absence of poly-grains and the relatively low TD density
relative to the other samples. This indicates that the growth
the wave pattern decreases, the height difference decreases.
It is assumed that this is the cause of the enhanced
surface roughness. Figures 5(a and b) show the (002),
(102) –2 rocking curves for each condition employed,
obtained by HR-XRD. The density of screw type (DS )
and edge type (DE ) dislocations can be estimated from the
full width at half maximum (FWHM) using the following
formulas:18
19
2s 2
Ds = = (1)
2 ln 2 × bs 2 435 ×
bs cos 2
Delivered bypattern
of poly-grains on the cone-shaped Ingenta to: Statethe
influences University of New York atBinghamton
2 2
102 − 2
002
E =
areThu, 18 MayD2017 =
e
TD. The surface roughness of theIP: 95.181.217.73
samples A, B, and C On: 06:39:18 (2)
Copyright: American 2 ln 2 × be 2 435 ×
be sin 2
shown more clearly in the AFM images (5 m × 5 m) Scientific Publishers
in Figures 4(a–c). Theses samples show wave patterns on where bs  and be  are the Burgers vector sizes of
the surface. In general, the GaN films form a wave pat- the screw TD (bs  = 0.5185 nm) and edge TD (be  =
tern on the surface that relaxes the stress due to the lattice 0.3189 nm), respectively. s and e were estimated using
mismatch between the films and substrate. As the amount the method outlined previously by Lee et al.20
of poly-grains on the cone-shaped pattern decreases, the

surface roughness decreases. The interval of the wave pat- 
h0l =
s cos 2 +
e sin 2 (3)
tern on the surface follows the same trend as the root
mean square (RMS) roughness. The RMS roughness val-
ues for samples A, B and C were 0.547 nm, 0.469 nm, and
002 and 
102 are
0.169 nm, respectively. Consequently, as the interval of
Here,  is the angle between the reciprocal lattice vector
(Khkl ) and the (001) surface normal. 
the HR-XRD FWHM values for the (002) and (102) peaks.

Figure 5. (a) (002) and (b) (102) omega rocking curves of the epitaxial GaN films grown on PSS under different conditions.

11578 J. Nanosci. Nanotechnol. 16, 11575–11579, 2016

Kim et al. Improvement of Epitaxial GaN Films Grown on Patterned Sapphire Substrate by Growth Mode Control

Table II. Experimental results from rocking curves from HR-XRD  growth rate of crystal surfaces by simply adjusting the
scans, indicating calculated screw-, edge-type dislocation densities for
growth temperature and pressure. The epitaxial GaN films
samples A–C.
grown on PSS via optimized growth mode control exhibit
Dislocation enhanced crystal quality and surface roughness. Overall,
FWHM (arcsec) density (108 cm−2  the method of controlling the growth mode can be widely
Sample 002 102 Screw-type Edge-type applied to the growth of single crystal thin films using
MO-CVD as well as to the growth of epitaxial GaN films.
A (condition I) 337.7 352.2 2.30 1.10
B (condition II) 260.1 352.9 1.36 6.42 In this way, it is possible to maximize the material proper-
C (condition III) 233.3 320.1 1.09 5.41 ties via simple morphological changes during the growth
process. This is a very promising technique for the pro-
The calculated TD densities are listed in Table II. The DS duction of high-quality thin films with no additional cost.
of the sample A was estimated to be 2.3 × 108 cm−2 .
This sample had the highest value, whereas the DE References and Notes
of this sample was the lowest due to the small interval 1. S. Nakamura, T. Mukai, and M. Senoh, Appl. Phys. Lett. 64, 1687
between the (002) and (102) FWHM values. The DS of (1994).
sample C was estimated to be 1.1 × 108 cm−2 , which is 2. S. Nakamura, M. Senoh, N. Iwasa, and S. Nagahama, Jpn. J. Appl.
Phys. 34, L797 (1995).
the lowest value for the evaluated samples. As the FWHM
3. I. Akasaki, S. Sota, H. Sakai, T. Tanaka, M. Koike, and H. Amano,
values of the (002) peak decreases, the DS decreases. This Electron Lett. 32, 1105 (1996).
result coincided exactly with the observations for the dark 4. S. Nakamura, M. Senoh, S. Nagahama, N. Iwasa, T. Yamada,
spots in the panchromatic CL images. Therefore, it was T. Matsuchita, H. Kiyoku, Y. Sugimoto, T. Kozai, H. Umemoto,
possible to improve the crystal quality of epitaxial GaN M. Sano, and K. Chocho, Jpn. J. Appl. Phys. 36, L1568 (1997).
5. X. A. Cao, J. M. Teetsov, M. P. D’Evelyn, D. W. Merfeld, and C. H.
films on PSS by only controlling the growth mode.
Yan, Appl. Phys. Lett. 85, 7 (2004).
6. M. Iwaya, T. Takeuchi, S. Yamaguchi, C. Wetzel, H. Amano, and
I. Akasaki, Jpn. J. Appl. Phys. 37, L316 (1998).
4. CONCLUSION
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In this paper, we report a method for obtaining high- 8. C. H. Chiu, H. H. Yen, C. L. Chao, Z. Y. Li, P. Yu, H. C. Kuo,
quality epitaxial GaN films on PSS by controlling the T. C. Lu, S. C. Wang, K. M. Lau, and S. J. Cheng, Appl. Phys. Lett.
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New (2008).
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Received: 27 November 2015. Accepted: 30 March 2016.

J. Nanosci. Nanotechnol. 16, 11575–11579, 2016 11579