ARTICLE IN PRESS

Physica B 382 (2006) 1720

www.elsevier.com/locate/physb

Epitaxial growth of ZnO lms by

helicon-wave-plasma-assisted sputtering
Guangsheng Fu, Heju Xu, Shufang Wang, Wei Yu, Wei Sun, Li Han
College of Physical Science and Technology, Hebei University, Baoding 071002, China
Received 13 December 2005; received in revised form 17 January 2006; accepted 19 January 2006

Abstract
The epitaxial growth of ZnO lms on Al2O3 (0 0 0 1) substrates have been achieved at a low-substrate temperature of 400 1C by using a
helicon wave-plasma-assisted sputtering technique. X-ray diffraction y2y scan, o scan and f scan indicate that the ZnO lms have a
good c-axis orientation and in-plane epitaxy. The photoluminescence measurement of the lms shows that there is only a strong emission
peak at 384 nm, and no visible emission related to the structural defects can be detected. A strong absorption in the ultraviolet region and
a high transparence of over 85% in visible region are obtained from the optical absorption measurements. Hall-effect measurement
reveals that the mobility of the deposited lms is 5.0 cm2/V.s. All above results demonstrate that this newly developed sputtering
technique provides a exible and powerful technique for the growth of high-quality epitaxial ZnO lms.
r 2006 Elsevier B.V. All rights reserved.
PACS: 81.05.Dz; 81.15.
z; 81.15.Cd
Keywords: ZnO lms; Epitaxy; Helicon wave plasma; Sputtering

1. Introduction
ZnO epitaxial lms have recently attracted great attention due to its potential applications in electrical and
optical devices [1,2]. Many techniques such as laser
molecular beam epitaxy (L-MBE) [3], metalorganic chemical vapor deposition (MOCVD) [4], pulsed laser deposition
(PLD) [5] and sputtering (radio frequency magnetron
sputtering and reactive sputtering) [6,7] have been used
for epitaxial growth of ZnO lms. Among these techniques,
sputtering was considered to be one of the most promising
methods for the fabrication of epitaxial lms because of its
low cost, simplicity, and low operating temperature.
However, the high-energy sputtering particles accelerated
by high bias voltage between the target and the substrate in
the sputtering chamber will lead to the surface damage of
the deposited lms. To overcome this problem, a new type
Corresponding author.
Also to be corresponded to.

E-mail addresses: w_yu_hbu@yahoo.com.cn, wsf@aphy.iphy.ac.cn

(S. Wang).
0921-4526/$ - see front matter r 2006 Elsevier B.V. All rights reserved.
doi:10.1016/j.physb.2006.01.535

of sputtering techniquehelicon wave plasma (HWP)

sputtering was proposed by Chichibu et al. [810].
Compared to conventional plasma sources, HWP has
many advantages including the higher plasma density,
lower ion energy and lower working pressure, which can
make the sputtering process operating at relatively low bias
voltage and decrease the deposition temperature. Furthermore, the HWP can be excited apart from the deposition
chamber, which is protable to control the gas phase and
surface reactions independently.
In this paper, we report the epitaxial growth of highquality ZnO lms on Al2O3 (0 0 0 1) substrares by using the
HWP-assisted sputtering technique at a low substrate
temperature of 400 1C. In this newly developed sputtering
technique, the high-density HWP can maintain the
sputtering process at a relative low bias voltage and can
activate the reactant gas more effectively. Furthermore, the
low ion kinetic energy of the HWP can enhance the
mobility of the precursors on the lm-growing surface,
which lead to a decrease of the lm deposition temperature.
X-ray diffraction (XRD) y2y scan, o-scan and f scans
reveal that the deposited ZnO lms have a good c-axis

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G. Fu et al. / Physica B 382 (2006) 1720

2. Experimental details

3. Results and discussion

Fig. 2 shows the typical XRD y2y scan and o-scan
measurement of an as-grown ZnO lm about 350 nm thick.
Only the (000 l) reections appear in the y2y scan,
indicating that the as-grown lm has its c-axis normal to
the substrate surface. The o-scan measurement of the ZnO
(0 0 0 2) reection reveal that the full-width at halfmaximum (FWHM) is less than 0.71, which indicates a
good c-axis orientation of the ZnO lm. XRD f scans
studies have been done to understand the quality of the
epitaxy and to determine the in-plane relationship between
the ZnO lms and the Al2O3 (0 0 0 1) substrates. The sixfold
symmetry reections from the f scans can be clearly seen in

the Fig. 3. A small FWHM value of f scans (Df1013
2:0 )
have been obtained, suggesting that the lms are high
degree in-plane orientation. These values are comparable
with those of the ZnO lms deposited by other techniques
[11,12]. The in-plane orientation relationship has been
determined to be (0 0 0 1) ZnO//(0 0 0 1)Al2O3.
The PL spectrum of the as-grown ZnO lms is measured
at room temperature, as shown in Fig. 4. A strong peak at
384 nm with the FWHM of about 12 nm can be seen, which
corresponds to the band-edge emission of the ZnO due to
the free exciton. No visible emission derived from the
structural defects is observed, and the emissions at 440 and
470 nm are the noises of the measurement apparatus. These
results reveal that the ZnO lms deposited by this newly
developed HWP-assisted sputtering technique have a very
few structural defects. The good optical characteristic of

Intensity (arb. units)

A schematic diagram of the HWP-assisted sputtering

apparatus developed by us is shown in Fig. 1, which is
some different from the apparatus reported by Chichibu et
al. [10]. The apparatus consists of a stainless-steel cylinder
chamber for the lm deposition and an upper quartz tube
as the plasma generation source. The base pressure was
5  10
3 Pa. The HWP was excited by a 30-MHz radio
frequency (RF) wave eld in the quartz tube with a 6-cmdiameter Nagoya III type external helicon antenna. The
static magnetic mirror was provided by the two electromagnetic coils surrounding the quartz tube. A magnetic
sputter cathode xed with a 99.99% pure ZnO wafer was
perpendicular to the quartz tube and was biased with
13.56 MHz RF power. The substrate was about 4 cm below
the sputtering target. In order to reduce oxygen vacancies
and zinc interstices in the deposited lms, a mixture gas of
Ar and O2 was used as reactant gas and was introduced
into the plasma generation source through mass ow
controllers. The ZnO lms were deposited at working
pressure of 0.6 Pa. The substrate temperature was kept at
400 1C. To maintain HWP, the static magnetic eld and RF
power were maintained at 200 G and 380 W, respectively.
The RF power imported to sputtering target was 80 W.
The crystalline structure of the deposited lms was
characterized by XRD y2y scan and o-scan, and the in-

plane epitaxial information was analyzed by f scans. The

optical qualities of the lms were obtained through the PL
spectrum and ultraviolet (UV)-visible absorption spectroscopy. The electrical properties were measured by Halleffect measurement.

Intensity (arb. units)

orientation and in-plane epitaxy. The measurement results

of photoluminescence (PL) spectrum and optical transmittance spectra of the deposited ZnO lms indicate the lms
have good optical quality.

ZnO(0002)

18

ZnO(0004)

13 14 15 16 17 18 19 20
(degree)

20

Fig. 1. A schematic diagram of the HWP-assisted sputtering system.

30

40

50
2 (degree)

60

70

80

Fig. 2. A typical XRD y2y scan of ZnO lms on Al2O3 (0 0 0 1)

subatrates. The inset is the o-scan measurement of the ZnO (0 0 0 2).

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G. Fu et al. / Physica B 382 (2006) 1720

100

Transmission (%)

ZnO (1013)

Intensity (arb. units)

19

Al2O3 (1123)

80

60

40

20

50

100

150
200
(degree)

250

300

400

350

500

600
700
wavelength (nm)

800

Fig. 5. Optical transmittance spectra of the epitaxial ZnO lms.

Fig. 3. XRD j scan patterns for the ZnO(1 0 1 3) diffraction and

Al2O3(1 1 2 3) diffraction.

intensity (arb. units)

contact between electrodes and lms was conrmed. The

measurements show that the sputtered ZnO lms exhibit ntype conduction. The electrical resistivity, the carrier
concentration and the mobility are 0.24 O cm
1,
1.3  1018 cm
3, and 5.0 cm2/V.s, respectively, which is
compared with those of the ZnO lms deposited by other
techniques [1315].

360

4. Conclusions

400

440
wavelength (nm)

480

520

Fig. 4. PL spectrum at room temperature of the epitaxial ZnO lms.

the lms indicates that these HWP-assisted sputtered ZnO

lms can be used in ultraviolet light-emitting devices and
novel interpreted optoelectronic devices.
The high quality of our ZnO lms was also conrmed
using the absorption spectra. Fig. 5 presents the UVvisible
absorption spectra of the ZnO lms epitaxied by the HWPassisted sputtering. It shows a sharp fundamental absorption edge at about 380 nm, indicating high quality of the asgrown ZnO lms. In the visible region, the lms are highly
transparent with the transmittance is over 85% and even
up to 100% in some wavelength region. The high
transmittance indicates that oxygen defects in our samples
are very few.
The electrical resistivity, carrier concentration, and
mobility of the as-grown ZnO lms were obtained by the
four-probe van the Pauw method using Hall-effect
measurement. Before electrical measurements, silver spot
electrodes were made on the ZnO lms and the Ohmic

In conclusion, high-quality ZnO epitaxial lms have

been successfully fabricated at the substrates of Al2O3
(0 0 0 1) at 400 1C by using a new-developed HWP-assisted
sputtering technique. Detailed XRD analysis indicate that
the deposited ZnO lms have a highly c-axis orientation
and in-plane epitaxy, while the measurements of PL
spectrum and the optical transmittance spectra reveal the
lms have good optical quality. Our results indicate that
the HWP-assisted sputtering method provides a exible
and powerful technique for the growth of high-quality
epitaxial ZnO lms.
Acknowledgments
This research was supported by the Natural Science
Foundation of Hebei Province, P R China (Grant no.
E2004000119).
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