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15 JUNE 2004
use of helicon-wave-excited plasma HWP, of which physics and experiments have been reported in early 90s,2023 as
a sort of remote plasma source for the sputtering deposition
of semiconductor thin films. As the first step, very smooth,
highly 0001-oriented, low-resistivity (5104 cm), and
transparent Al-doped ZnO thin films have been deposited on
the glass substrate without additional annealing in oxygen
ambient.19 These achievements are due to the properties of
HWP, which can be excited under relatively higher vacuum
(104 Torr) producing a high density and lower ion energy
plasma. Subsequently, completely a-axis-locked six-fold
0001 orientation ZnO epilayers have been grown on
(0001) Al2 O3 substrates.24 According to the achievement of
near-band-edge emission at room temperature from the epilayers due to the surface-damage-free nature, the technique
was named helicon-wave-excited-plasma sputtering epitaxy HWPSE.24 The atomic species responsible for the
film growth during HWPSE of ZnO was recently found by in
situ sputtered-plume emission spectroscopy measurements25
to be excited neutral Zn Zn*, as well as nonradiative species such as molecular ZnO. Since the growth rate was
limited by the sticking coefficient of Zn, the growth mode of
HWPSE was concluded to be similar to that of LMBE.25
Therefore, a proper technique to control the initial stage of
the growth such as surface arrangements as well as lattice
matching is considered to be important.
ZnO has a band gap energy of 3.37 eV, and has a wurtzite crystal structure with the a lattice parameter of 3.250 .
The relation between the band gap energies and in-plane lattice parameters a of ZnO, MgO, CdO, and Al,In,GaN semiconductors is summarized in Fig. 1a. ZnO films have been
usually grown on 0001 face of Al2 O3 substrates, because
I. INTRODUCTION
0021-8979/2004/95(12)/7856/6/$22.00
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II. EXPERIMENT
FIG. 1. a Energy gap E g vs a-lattice parameter of ZnO, MgO, CdO, and
Al, In, GaN semiconductors. Equivalent lattice parameters of 0001 and
0) Al O are also shown by vertical broken lines. Epitaxial relation(112
2 3
0) Al O . For simplicity, Zn
ships of 0001 ZnO on b 0001 and c (112
2 3
0) Al O substrate are
atoms in the ZnO epilayer and O atoms in the (112
2 3
selectively shown in c.
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7858
In XRD measurements, mosaicity, compositional variation, and strain distribution can be analyzed separately. Two
popular scans, namely scan rocking scan and 2 scan
are conventionally used to evaluate the crystalline mosaicity
and the distribution of out-plane lattice constant, respectively. A mosaic crystal is defined as an ensemble of perfect
crystal blocks, whose sizes vary around a mean value, with
lattice planes tilted with respect to each other. The mosaicity
in the hexagonal crystal can be divided into two portions;
i.e., tilting misorientation in c-axis and twisting misorien-
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7859
0 ZnO 112
0 AlN(4.4%)
relations
and
112
results imply the presence of high-density dislocations having an edge component33 in ZnO/0001 AlN. Combined
with the result that ZnO/0001 AlN exhibited the largest
FWHM value for the rocking curve, the epilayer is considered to contain very high density dislocations as well as
orientation-domain boundaries, although the lattice and thermal expansion mismatches between ZnO and AlN are
smaller than those between ZnO and Al2 O3 . One of the rea-
TABLE I. Lattice mismatch, epitaxial relations, FWHM values of XRD peaks, and FWHM values of the
near-band-edge PL peak at 293 K for the ZnO epilayers grown by HWPSE.
ZnO/(0001) Al2 O3
0) Al O
ZnO/(112
2 3
ZnO/0001 AlN
0)
(0001) ZnO (112
Al2 O3
and
0) (0001)
(112
ZnO
Al2 O3
0.08
0002 2 deg.b
0002 deg.b
3) deg.b
(101
0.19
0.66
2.57
0.13
0.48
1.37
0.18
1.10
3.03
Surface morphology
Rough
with
precipitates
Smooth with
0.26-nm-high
monolayer steps
Rough
with
precipitates
153
107
124
Structure
Epitaxial relations
In-plane lattice
Mismatch %a
4.4
9.7 30 rotated
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7860
0) Al O , and
FIG. 5. PL spectra of a ZnO/(0001) Al2 O3 , b ZnO/(112
2 3
c ZnO/0001 AlN measured at 293 K.
0) Al O substrate
FIG. 4. a AFM image of the ZnO film grown on a (112
2 3
and SEM bird view images of b ZnO/(0001) Al2 O3 , c
0) Al O , and d ZnO/0001 AlN. A cross-sectional height proZnO/(112
2 3
0) Al O grown at 700 C is also shown. The step height of
file of ZnO/(112
2 3
0.26 nm corresponds to a half of the c-lattice parameter.
sons for the formation of high density dislocations and multidomains is considered to be the presence of Al
suboxynitrides at the ZnO/AlN interface due to the natural
oxidation of the AlN surface, since the pregrowth surface
treatment of AlN is in principle difficult and the overlayer
ZnO contains oxygen in the matrix. Another possibility is
the formation of polycrystalline spinel ZnAl2 O4 , whose
a-axis length is 0.80848 nm, at the ZnO/AlN interface.34
Moreover, the formation of inversion domains is probable,
since most of IIInitride epilayers grown by MOVPE grow
toward the 0001 face group-III polarity35,36 while ZnO
)
epilayers grown by LMBE in usual grow toward the (0001
37
face O polarity. Therefore, a proper purification technique
for the AlN surface or the insertion of an appropriate buffer
layer is necessary to form a single-domain ZnO/AlN heterointerface.
B. Surface morphology and PL spectra
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that between (1120) ZnO and (1010) Al2 O3 . The result suggested the formation of interfacial suboxynitrides, ZnAl2 O4
spinels, or inversion domains. Proper purification processes
for the AlN surface or the insertion of appropriate buffer
layers are required to form single-domain heterovalent ZnO/
AlN interfaces. Achievements of the atomically flat 2D terraces, excitonic features in the low-temperature optical spectra, and a predominant near-band-edge PL peak FWHM
107 meV at room temperature in the ZnO epilayer grown
0) Al O substrate indicate that HWPSE can be
on the (112
2 3
regarded as one of the promising epitaxial growth techniques
to fabricate high-quality ultrathin quantum structures having
atomically abrupt heterointerfaces for future device applications.
ACKNOWLEDGMENTS
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