Novel metalorganic chemical vapor deposition system for GaN growth

Shuji Nakamura, Yasuhiro Harada, and Masayuki Seno

Citation: Appl. Phys. Lett. 58, 2021 (1991); doi: 10.1063/1.105239

View online: http://dx.doi.org/10.1063/1.105239
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Published by the American Institute of Physics.

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 Novel metalorganic chemical vapor deposition system for GaN growth
Shuji Nakamura, Yasuhiro Harada, and Masayuki Seno
Nichia Chemical Industries Ltd., 491 Oka, Kaminaka, Anan, Tokushima 774, Japan
(Received 28 September 1990; accepted for publication 10 February 1991)
A novel metalorganic chemical vapor deposition (MOCVD) system, which has two different
flows, has been developed. One flow carries a reactant gas parallel to the substrate, and
the other an inactive gas perpendicular to the substrate for the purpose of changing the
direction of the reactant gas flow. The growth of a GaN film was attempted using this
system, and a high quality, uniform film was obtained over a 2 in. sapphire substrate. The
carrier concentration and Hall mobility are 1 x 10’* /cm3 and 200 cm2/V s, respectively,
which are the highest for GaN films grown directly on a sapphire substrate by the MOCVD
method.

Gallium nitride (GaN) is one of the most potential
materials which can be used as a wide-gap semiconductor
with applications for blue, violet, and ultraviolet light-
emitting devices. For the fabrication of these optical de-
vices, high quality GaN film is required. Usually, GaN film
is grown on a sapphire substrate by the metalorganic
chemical vapor deposition (MOCVD) method, and the
grown layers usually show n-type conduction without any
intentional doping. Recently, much progress has been
achieved in the crystal quality of GaN film. Carrier con-
centration and Hall mobility, whose values were (2-
5) X 10”/cm3 and 350-430 cm2/V s, were obtained by the
prior deposition of a thin AlN layer as a buffer layer before
the growth of GaN filrn.le3 However, without the AlN
buffer layer, the carrier concentration was around 2 X 1019/
cm3 and the Hall mobility was only around 50 cm2/V s in
MOCVD growth without any intentional doping. To form
a high quality film for the fabrication of optical devices,
these values must be improved. In the previous investiga-
tions, a thin delivery tube was used to feed a reactant gas to
the substrate for the purpose of obtaining a high gas veloc-
N2+H2
CONICAL
yJgT2
4IR RADIATION
THERMOMETER
STAINLESS
@I-CC, II I N2+ H2
ity (around 5 m/s).tm5 For this reason, it was very difficult
to get a high quality film uniformly over the sapphire sub-
strate.
A novel MOCVD reactor, which is shown in Fig. 1,
was developedfor the GaN growth. It has two different gas
flows. One is the main flow which carries the reactant gas
parallel to the substrate with a high velocity through the
quartz nozzle. Another flow is the subflow which trans-
ports the inactive gas perpendicular to the substrate for the
purpose of changing the direction of the main flow to bring
the reactant gas into contact with the substrate (see Fig.
2). This subflow is very important. Without the subflow, a
continuous film was not obtained and only few island
growths were obtained on the substrate. The mixed gas of
H, and N, was used as the subflow. We call this system a
two-flow MOCVD (TF-MOCVD). The growth of GaN
film was operated at atmospheric pressure. Sapphire with
(0001) orientation (C face) was used as a substrate. Tri-
nethylgallium (TMG) and ammonia (NH3) were used as
Ga and N sources, respectively. First, the substrate was
heated at 1050“C in a stream of hydrogen. Then, the sub-
strate temperature was lowered to 1000 “C to grow the
GaN film. During the deposition, the flow rates of H,,
NH,, and TMG of the main flow were kept at 1.0 &min,
5.0 &min, and 54 pmol/min, respectively. The flow rates
of H, and N, of the subflow were kept at 10 and 10 e/min,
SUBFLOW

;f$f!;ETEu L 1~ H2 +NH3 +TMG

MAIN FLOW
TMG + NH3+ H2
SUSCEPTOR

_..-_--.

FIG. I. Schematicnovel MOCVD reactorfor GaN growth. FIG. 2. Schematicprinciplefigureof two-flowMOCVD.

2021 Appt. Phys. Lett. 58 (18), 6 May 1991 0003-6951191 /182021-03$02.00 @ 1991 American Institute of Physics 2021
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 D 25 = lo3 2
2
3

(a) -loo pm - ,g
- .-
:I0 g
FIG. 3. Interferencemicrographsof the surfaceof the grown GaN film;
(a) sampleA, (b) sampleB.
w- Distance (mm)
15 20 25

respectively. The growth time was 40 min. This sample was

labeled sample A. Its thickness was about 3.0 pm. Another
sample was labeled sample B, which was grown under the
samecondition as sample A except the flow rates of H, and
N2 of the subflow, which were changed to 10 and 0 flmin,
respectively. The thickness of sample B was about 2.5 ,um.
Figure 3 shows the surface morphology of the grown
GaN film. Normal hexagonal-like pyramid growths are ob-
served on the surface of sample A. Many small distorted
hexagonal-like pyramid growths are observed on the sur-
face of sample B. Therefore, the surface morphology of the
GaN film is affected by the flow rate of the subflow in this
TF-MOCVD system. Figure 4 shows the thickness distri-
bution of sample A. Good uniformity is obtained around
the center. Hall measurement was performed by the van
der Pauw method at room temperature. The results of sam-
ple A are shown in Fig. 5. The carrier concentration and
Hall mobility are 1 x 10”/cm3 and 200 cm2/V s, respec-
tively. The distribution of the carrier concentration and the
Hall mobility shows good uniformity. The value of the
FIG. 5. Distribution of the carrier concentrationand the Hall mobility.
Hall mobility is the highest one for GaN films grown di-
rectly on the sapph.iresubstrate. The carrier concentration
and the Hall mobiltity of sample B were 1 X 1019/cm3and
40 cm’/ V s, respectively. The crystal quality of the GaN
film was characterized by the double-crystal x-ray rocking
curve (XRC) method. The full width at half maximum
(FWHM) for (0002) diffraction from the GaN film of
sampIe A is shown in Fig. 6. These values, about 5 min, are
much better than ordinary values (about 8 min) obtained
through the conventional MOCVD method. The FWHM
of sample B is about 40 min.
In the TF-MOCVD system, the reactant gas flows par-
allel to the substrate. Thus, the lateral growth rate in the
GaN growth by this system is larger in comparison with
that by the conventional MOCVD system in which the
reactant gas Rows perpendicular or diagonally to the sub-
strate, A continuous film is easily obtained by the present
method. Also the crystal quality of the GaN film is im-
proved.

3.5
10
-1 3.0
g 00.0 .**w
2 0

8 2.0 l
3 2.5 .:. 00

-25 0 25
1.5 e
7‘
-I
\ 0 25 0 5 10 15 20 25
Distance(mm) Distance(mm)
FIG. 4. Distribution of the thicknessof the GaN film. FIG. 6. Distribution of the FWHM of the XRC for (ooO2)diffraction.

2022 Appt. Phys. Left., Vol. 58, No. 18, 6 May 1991 Nakamura, Harada, and Seno 2022

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 In summary, a novel MOCVD system, which has two *H. Amano, I. Akasaki,K. Hiramatsu,and N. Koide, Thin Solid Films
different flows, was developed. High quality, uniform GaN 163,415 (1988).
H
‘ . Amano,M. Kito, K. Hiramatsu,and I. Akasaki,Jpn. J. Appl. Phys.
film was obtained on a 2 in. sapphire substrate using this 28, L2112 (1989).
system. 4M. Hashimoto, H. Amano, N. Sawaki, and I. Akasaki, J. Cryst.
Growth. 68, 163 (1984).
’ H. Amano,N. Sawaki,I. Akasaki,and Y. Toyoda,Appl. Phys.Lett. 48, Y
‘ . Koide, H. Itoh, N. Sawaki,and I. Akasaki,J. Electrochem.Sot. 133,
353 (1986). 1956(1986).

Publishedwithout authorcorrections

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