Synthesis and characterization of ZnO thin film grown by electron beam evaporation

D. C. Agarwal, R. S. Chauhan, Amit Kumar, D. Kabiraj, F. Singh, S. A. Khan, D. K. Avasthi, J. C. Pivin, M. Kumar
, J. Ghatak, and P. V. Satyam

Citation: Journal of Applied Physics 99, 123105 (2006); doi: 10.1063/1.2204333

View online: http://dx.doi.org/10.1063/1.2204333
View Table of Contents: http://scitation.aip.org/content/aip/journal/jap/99/12?ver=pdfcov
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 JOURNAL OF APPLIED PHYSICS 99, 123105 共2006兲

Synthesis and characterization of ZnO thin film grown by electron

beam evaporation
D. C. Agarwala兲 and R. S. Chauhan
Department of Physics, R. B. S. College, Agra 282 002, India
Amit Kumar, D. Kabiraj, F. Singh, S. A. Khan, and D. K. Avasthi
Inter-University Accelerator Centre, P.O. Box 10502, New Delhi 110 067, India
J. C. Pivin
CSNSM, IN2P3-CNRS, Batiment 108, F-91405 Orsay Campus, France
M. Kumar
Department of Physics, Allahabad University, Allahabad 211 002, India
J. Ghatak and P. V. Satyam
Institute of Physics, Sachivalaya Marg, Bhubanashwar 751 005, India
共Received 28 November 2005; accepted 16 April 2006; published online 22 June 2006兲
Highly transparent, conducting, highly oriented, and almost single phase ZnO films have been
deposited by simple e-beam evaporation method, and the deposition parameters were optimized.
The films were prepared by 共a兲 evaporation of ZnO at different substrate temperatures and 共b兲
evaporation of ZnO at room temperature and subsequent annealing of the films in oxygen ambient
at different temperatures. The characterizations of the film were performed by optical absorption
spectroscopy 共UV-visible兲, Fourier transform infrared spectroscopy, resistivity measurement,
transmission electron microscopy 共TEM兲, photoluminescence, and x-ray diffraction measurement.
Absorption spectra revealed that the films were highly transparent and the band gap of the pre- and
postannealed films was in good agreement with the reported values. The band gap of the films
increases on increasing the substrate temperature as well as annealing temperature, whereas the
resistivity of the film decreases with substrate temperature and increases with annealing
temperature. Fourier transform infrared spectroscopy of ZnO films confirms the presence of Zn–O
bonding. X-ray diffraction, electron diffraction, and TEM images with high resolution and Raman
spectra of the films showed the formation of crystalline ZnO having wurtzite structure. © 2006
American Institute of Physics. 关DOI: 10.1063/1.2204333兴

I. INTRODUCTION used indium-doped tin oxide 共ITO兲 transparent electrodes

The semiconductors Si and Ge based electronic devices
cannot be used at high temperature due to small band gap of
these materials. Therefore, wider band gap semiconductors
are required for high temperature devices. Transparent semi-
conducting ZnO thin films have attracted considerable atten-
tion from both fundamental and application points of view,
primarily because of their useful properties. Zinc oxide is
n-type semiconductor of wide interest exhibiting excellent
optical, electrical, catalytic, gas sensing properties and has
great technological applications in various fields.1–6 The no-
table properties of ZnO are its wide band gap of 3.3 eV at
room temperature and high exciton binding energy 共60 meV兲
compared to those of ZnS 共20 meV兲 and GaN 共21 meV兲.7–11
Due to its wide band gap, ZnO can be used for short wave-
length light emitting devices such as light emitting diodes
and laser diodes, surface acoustic wave 共SAW兲 bandpass fil-
ters, optical waveguides, and laser deflectors using piezo-
electric or piezo-optic properties. It is also used in gas sen-
sors, varistor, and as transparent conducting oxide. ZnO has
proved to be an interesting alternative for the commonly
a兲
Author to whom correspondence should be addressed;
dcagarwal@gmail.com
owing to lower absorption in UV, higher stability in hydro-
gen plasma, lower cost and higher availability, and lack of
toxicity. Hence ZnO is useful material for optoelectronics
applications because it exhibits semiconducting as well as
piezoelectric properties.
ZnO films can be deposited by a variety of techniques,
such as sol-gel chemistry,12 spray pyrolysis,13 metal organic
chemical vapor deposition,14 molecular beam epitaxy,11
pulsed laser deposition,15,16 reactive thermal evaporation,17
and sputtering.18 The properties of grown thin films and in-
terfaces depend on the deposition process and deposition pa-
rameters. Every deposition technique has its own advantages
and disadvantages. Thermal evaporation is widely used and
well-known technique generally to deposit films with
smoother surface than other techniques and less or no dam-
age at the substrate interface. Sufficiently conducting ZnO
films for device application can be obtained by e-beam
evaporation process with controlled conditions and subse-
quent annealing. The ZnO has a hexagonal-close-packed
wurtzite structure which shows a strong 具001典 preferred ori-
entation, perpendicular to the substrate, related to a mini-
mum of the surface energy.19 It is known that ZnO displays
three major PL peaks as mentioned in the literature: an UV

0021-8979/2006/99共12兲/123105/6/$23.00 99, 123105-1 © 2006 American Institute of Physics

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 123105-2 Agarwal et al. J. Appl. Phys. 99, 123105 共2006兲

near band-edge emission peak around 380 nm, a green emis- TABLE I. Summary of the sample codes and deposition conditions for the
sion around 510 nm, and a red emission around 650 nm.20 preparation of ZnO films with band gap and resistivity.
Band-edge emission is sharp and strong while the other two
Annealing
emissions are weak and broad. Normally ZnO thin films Sample Substrate temperature temperature Band gap Resistivity
show n-type conduction due to oxygen vacancies and inter- identity 共°C兲 共°C兲 共eV兲 共⍀ cm兲
stitial Zn ions which act as donors in the ZnO lattice. The red
Z0 Room temperature No 1.51 14.65⫻ 10−2
and green emissions are attributed to oxygen vacancies and
Z1 100 No 3.08 12.1⫻ 10−2
Zn ions in the interstitial position. In most polycrystalline Z2 200 No 3.13 4.70⫻ 10−2
thin films, defect related deep level emissions dominate the Z3 300 No 3.22 3.65⫻ 10−2
PL spectra, which precludes various applications such as UV Z4 400 No 3.26 2.54⫻ 10−2
luminescent devices and unconventional polycrystalline lay- Z5 Room temperature 450 3.18 9.7
ers, known as “random laser” recently demonstrated in poly- Z6 Room temperature 600 3.22 28
crystalline ZnO thin films.21,22 Because the center energy of Z7 Room temperature 800 3.26 86
the green, yellow, and orange emissions is smaller than the
band gap energy of ZnO film, these emissions must be re-
lated to a localized deep level in the band gap. The origin of Mechelle 900 monochromator system with a Si charge
the defect related deep level photoluminescence 共PL兲 band coupled detector was used in measurements. Optical absorp-
has been investigated for a long time. However, due to the tion spectra were recorded with the conventional two-beam
complexity of the microstructure of ZnO, there is still no method using U-3300 UV-VIS spectrophotometer of Hitachi.
satisfactory consensus.22–24 Large exciton energy and good The Zn–O bonding and vibrational modes were studied by
luminescence properties make the ZnO useful for optical ap- Fourier transform infrared spectroscopy 共FTIR兲 and Raman
plications. In the present work, a study on the defect emis- spectroscopy. The FTIR spectra were recorded in the range
sion in the thermally evaporated ZnO film and effect of post- of 400– 4000 cm−1, with a spectral resolution of 4 cm−1. The
annealing and substrate temperature on the structural, Raman spectra of the films were recorded using DILOR XY
optical, and electrical properties of the ZnO film is per- Raman spectrometer with spectral resolution of 1 cm−1 in
formed. CSNSM, Orsay. The nature of formed phases was studied by
means of TEM, electron diffraction, and x-ray diffraction
II. EXPERIMENTAL WORK 共XRD兲. The XRD spectra of ZnO films were recorded with
Brucker AXS x-ray diffractometer using Cu K␣ at IUAC,
A. Synthesis
New Delhi. High resolution transmission electron micros-
The ZnO thin films 共⬃100 nm兲 were deposited by ther- copy 共HRTEM兲 images of the ZnO film deposited at 300 ° C
mal evaporation of ZnO powder in the form of a pellet on were taken with a JEOL-2010-UHR instrument operated at
unheated Si and quartz. The substrates were washed with 200 kV at Institute of Physics 共IOP兲, Bhubaneswar. The
trichloroethylene, acetone, and alcohol. The distance from point to point resolution of HRTEM was 0.19 nm. The resis-
source to substrate and source to quartz crystal was of tivity measurements of the films at room temperature by the
15 cm. The vacuum before evaporation was of 5 ⫻ 10−7 torr, Vander-Pauw method were also measured at IUAC, New
during evaporation at room temperature was of 8 Delhi.
⫻ 10−6 torr, and during evaporation at higher substrate tem-
perature was of 6 ⫻ 10−5 torr. The deposition rate was
III. RESULTS AND DISCUSSION
0.1– 0.4 nm/ s. After deposition at RT, the films were black.
The black color may be due to the oxygen deficiency and A. XRD analysis
large number of defects. Therefore, these films were an- Figure 1共a兲 shows the x-ray diffraction spectra of ZnO
nealed in oxygen ambient at temperatures of 450, 600, and films deposited at different substrate temperatures. The film
800 ° C for 2 h. After annealing, the films were totally trans- Z0 showed polycrystalline nature, with 共100兲, 共002兲, and
parent. Films were also deposited on quartz, Si, and C-coated 共101兲 peaks of hexagonal ZnO at 31.75°, 34.35°, and 36.31°.
transmission electron microscopy 共TEM兲 grids keeping the As the substrate temperature is increased, the fiber texture
substrate temperature at 100, 200, 300, and 400 ° C. Other
deposition parameters were the same as described above. Af-
ter deposition the films were transparent. The summary of
the sample codes and deposition conditions for the prepara-
tion of ZnO films with band gap and resistivity is given in
Table I.

B. Sample characterization
Photoluminescence 共PL兲 and UV-VIS absorption mea-
surements were carried out to characterize the optical prop-
erties of films at Inter-University Accelerator Centre 共IUAC兲,
New Delhi. PL spectra were recorded under excitation with FIG. 1. XRD spectra of ZnO thin film 共a兲 at different substrate temperatures
the 325 nm line of He–Cd laser with a power of 27 mW. A and 共b兲 at different annealing temperatures.
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 123105-3 Agarwal et al. J. Appl. Phys. 99, 123105 共2006兲

along the c axis 共002兲 共peak at 34.43°兲 becomes the most

prominent peak while the other two peaks disappear. This
shows the improvement in the fiber texturing of the films
along the c axis with substrate temperature. The high sub-
strate temperature enables the atoms to move to their stable
orientation.25 A new peak 共103兲 has been observed at higher
substrate temperature of 300 ° C. The appearance of the
共103兲 orientation at higher temperature is due to some atoms
relocating at higher states because nuclei with this orienta-
tion become stable when providing thermal energy for com-
pensating this higher surface energy. The d value calculated
for the 共002兲 peak remains constant at around 0.264 nm with FIG. 2. ZnO film deposited at 300 ° C substrate temperature. 共a兲 HRTEM
increase in the substrate temperature from RT to 300 ° C. image, 共b兲 electron diffraction pattern.
Earlier reports indicated that the films deposited by dc mag-
netron sputtering at a substrate temperature of 323 K had a polar semiconductor with 共001兲 planes being Zn terminated
preferred orientation along the 共002兲 plane, a random orien-
and 共001̄兲 being O terminated. These two crystallographic
tation at 473– 573 K, and again a preferred orientation along
planes have opposite polarity and hence have different sur-
the 共002兲 crystal plane at 623– 753 K 共Refs. 26 and 27兲,
face relaxation energies, resulting in high growth rate along
whereas in the case of rf sputtered films it was noticed that
the c axis.28 The value of d spacing was calculated from the
the films formed at 313 K exhibited a mixed orientations
HRTEM image and electron diffraction pattern. The calcu-
while those formed at 473 K exhibited single phase of ZnO
lated values of d spacing for the 共002兲 plane are 0.269 and
with the 共002兲 orientation. The average grain sizes of the
0.271 nm, respectively, which are in good agreement with
films deposited at different substrate temperatures were cal-
XRD results.
culated using the Scherrer’s formula:
0.9␭
D= , 共1兲
␤ cos ␪
C. Raman spectroscopy
where ␭, ␤, and ␪ are x-ray wavelength 共1.541兲, full width of
half maximum 共FWHM兲 of the 共002兲 peak, and the Bragg The resulting Raman spectrum of Z3 film obtained at
diffraction angle. The average grain size of the films in- room temperature is shown in Fig. 3. The Raman active pho-
creases from 10.5 to 17 nm with increase in the substrate non modes for the wurtzite structure of ZnO expected from
temperature, as expected, due to the improvement in the the group theory are A1 + 2E2 + E1. The characteristic mode of
crystallinity of the films. Figure 1共b兲 shows the XRD pattern ZnO wurtzite phase at around 433 cm−1 共Ref. 29兲 is observed
of ZnO films deposited at RT and annealed in oxygen ambi- for ZnO films which also show prominent peak at 34.5° in
ent for 2 h at different temperatures. The XRD patterns for the XRD spectrum. Other than the characteristic mode of
the postannealed ZnO films indicated that they possess poly- ZnO, few second order modes are also observed. The modes
crystalline hexagonal wurtzite crystal structure with no pre- at 233 and 299 cm−1 are related to B1共high兲-B2共low兲 and the
ferred orientation. XRD spectra of the annealed films shows mode at 822 cm−1 is related to the B1共high兲 + B1共low兲 phonon
that the crystallinity of the film improves with increasing the mode frequencies.30 The peak at 630 cm−1 has been assigned
annealing temperature up to 600 ° C as the intensity of the to E1-LO mode.31 The E1-LO mode at phonon frequency of
共100兲, 共002兲, and 共101兲 peaks increases and FWHM de-
creases. When annealing temperature is further increased to
800 ° C, the intensity of the 共002兲 peak decreases due to the
deterioration of crystallinity in this orientation and the inten-
sity of the 共100兲 and 共101兲 peaks increased. The x-ray dif-
fraction studies revealed that the higher substrate tempera-
ture of 300 ° C is the optimum condition to generate highly
c-axis oriented zinc oxide films.

B. Transmission electron microscopy

In addition to the XRD analysis, we have also confirmed
the crystallinity of the film using TEM analysis. Films with
thickness of 50 nm were grown directly on carbon-coated
TEM grids. Figures 2共a兲 and 2共b兲 showed the HRTEM lattice
image and the electron diffraction patterns of ZnO film de-
posited at substrate temperature of 300 ° C. The electron dif-
fraction clearly demonstrated that the ZnO film grew along FIG. 3. Raman spectra of ZnO thin film deposited at 300 ° C substrate
the c axis which is consistent with the XRD results. ZnO is a temperature.
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 123105-4 Agarwal et al.
FIG. 4. 共a兲 FTIR spectra of ZnO thin film deposited at different conditions.
共b兲 Variation of FWHM of 408 peak of the ZnO thin film at different sub-
strate temperatures.
630 cm−1 was theoretically calculated by Zaoui and Sekkal
using the atomistic calculations based on an interatomic pair
potential with in the shell model approach.
D. FTIR spectra
FTIR was employed to reveal the Zn–O bonding. FTIR
spectra of ZnO films on Si substrate as shown in Fig. 4共a兲
show a strong peak at 408 cm−1 and two weak peaks at 513
and 567 cm−1. Andres-Verges et al.32 theoretically calculated
a strong IR band at 406 and one of small intensity at 580 for
slab-type ZnO particles 共c / a Ⰶ 1兲. Hayashi et al.33 also re-
corded the IR spectra of ZnO and compared them with the
calculated spectra. ZnO show three distinct absorption peaks
located between the bulk TO-phonon frequency 共␻T储兲 and
LO-phonon frequency 共␻L⬜兲. The present FTIR results are in
good agreement with the reported values, confirming the
ZnO phases over the whole temperature range. The peak at
408 cm−1 of the films deposited at different substrate tem-
peratures is fitted by Gaussian distribution. The FWHM of
the peak corresponding to the 408 cm−1 vibration decreases
with increase in the substrate temperature but no significant
change in the peak position is observed with the variation of
substrate temperature. The variation in FWHM of the peak
corresponding to the 408 cm−1 vibration, shown in Fig. 4共b兲,
shows that Z0 film has larger FWHM which indicates wider
distribution of vibrational energy of the ZnO molecule. As
substrate temperature is increased the FWHM decreases,
showing that distribution of vibrational energy becomes nar-
rower, indicating that the crystallinity of the film is improved
on increasing the substrate temperature. There are some re-
FIG. 5. Absorption spectra of ZnO thin film 共a兲 at different substrate tem-
peratures and 共b兲 at different annealing temperatures.
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J. Appl. Phys. 99, 123105 共2006兲
FIG. 6. Variation in band gap of ZnO thin films with substrate and annealing
temperatures.
ports available which show that the higher the FWHM of the
FTIR absorption peak, the smaller is the grain size.34,35 A
crystallinity can be defined from the damping constant36 共␥兲
which is defined according to the relation
1
T共w兲
−1=f
w
wTO
, 冉 冊 共2兲
where T共w兲 is the experimental transmittance and the
FWHM of the function f共w / wTO兲 is the measure of the
damping constant which defines the damping in optical vi-
brational modes and measure of crystallinity. The FWHM of
the peak at 408 cm−1 also decreases for the films Z5 – Z7,
giving a clue that the crystallinity increases on annealing of
the RT deposited samples.
E. Optical absorption study
The dependence of absorption of the films deposited on
quartz on wavelength is shown in Figs. 5共a兲 and 5共b兲. The
transmittance shows a strong temperature dependence. Films
deposited at room temperature 共RT兲 have a significant, con-
tinuous absorption in the visible range, demonstrating the
presence of a noticeable amount of metallic zinc and consid-
FIG. 7. PL spectra of ZnO thin film 共a兲 at different substrate temperatures
and 共b兲 at different annealing temperatures 共the intensity of the film grown at
RT and postannealed at 450 ° C was multiplied by 10兲.
 123105-5 Agarwal et al. J. Appl. Phys. 99, 123105 共2006兲

erable amount of defects in the RT deposited films. The me-

tallic zinc can be incorporated in the film as droplets or as
coherent domains of metallic zinc with zinc oxide. The band
edge becomes sharper on increasing the substrate tempera-
ture. The transmittance is poor in as-deposited state and it
increases with increasing the substrate temperature or post-
deposition annealing. The increase in the transmittance in the
films grown at higher substrate temperatures or in postan-
nealed films in oxygen is likely to be related, in part, to the
decrease in defects and increase in the ZnO to Zn ratio. The
absorption spectra of annealed films show sharper band edge,
as also those of ZnO films deposited on heated substrate. The
increase of transmittance is attributed to the intake of the
oxygen in the oxygen deficient ZnO films. The absorbed
oxygen removes the oxygen vacancies, hence reducing the
density of these donorlike defects. From the optical absorp-
tion spectra, the band gap of ZnO films is determined using
the Tauc’s procedure of plotting 共␣h␯兲2 vs h␯ and extrapo-
lating the linear portion of absorption edge to the energy
axis. The band gap of the films Z0 – Z7 was given in Table I.
FIG. 8. Variation of resistivity of ZnO thin films with substrate and anneal-
These values show that the band gap is small in films depos-
ing temperatures.
ited at room temperature and increases with increase in an-
nealing temperature or substrate temperature. The small band
gap in the case of deposition at RT may be attributed to the case, a broad peak at 575 nm is observed. No significant
energy levels in the intrinsic gap due to the defects such as change in the peak intensity is observed after annealing at
oxygen vacancies and Zn ions at the interstitial sites. The 450 ° C but peak position shifts at 552 nm. When film is
increase in band gap energy upon increasing the substrate annealed at 600 and 800 ° C, the intensity of the peak in-
temperature or annealing temperature is due to the decrease creases and shifts to 552 nm. Since the concentration of oxy-
in the amount of defects. gen vacancies and zinc interstitial ought to decrease with the
annealing of the film in oxygen ambient, the oxygen intersti-
tial 共Oi兲 and antisite oxygen OZn can be easily formed. Hence
F. Photoluminescence spectra the enhancement in the emission intensity is due to the in-
PL measurements were performed at room temperature crease of antisite oxygen 共OZn兲 and oxygen interstitial 共Oi兲.
with the 325 nm line of a continuous wave He–Cd laser. The
band-edge emission could not be observed because the used
filter of the laser light was cutting the wavelength less than
400 nm. PL spectra of ZnO films on Si deposited at different
G. Resistivity measurement
substrate temperatures are shown in Fig. 2共a兲. The film Z0
deposited at RT shows yellow emission centered around ZnO films deposited on any substrate exhibited n-type
570 nm. It is attributed to the transition between conduction conductivity,37 in which the electrical conductivity is due to
band to defects states or defects states to valence band. the excess zinc presumably located interstitially within the
Therefore, the intensity variation of the defect related emis- lattice and oxygen vacancies. Electrical resistivity of all films
sion may result from the variation of the intrinsic defects in was measured using the Vander-Pauw four-probe method at
ZnO film, such as zinc vacancy VZn, oxygen vacancy VO, room temperature. Various deposition conditions resulted in
interstitial zinc Zni, interstitial oxygen Oi, and antisite oxy- dramatic changes in film resistivity. The variation in resistiv-
gen OZn. This may be due to the presence of Zn interstitial ity with substrate temperature and annealing temperature is
and oxygen vacancies in the film. On increasing the substrate shown in Fig. 8. The resistivity of the film strongly depends
temperature, the intensity of the PL emission increases with upon the substrate temperature as well as annealing tempera-
redshift centered at 615 nm. This red PL is related with band ture. Resistivity of the film decreases with substrate tempera-
emission from deep interband levels, which are identified as ture and increases with annealing temperature. The decrease
oxygen vacancies or interstitial zinc. Since oxygen vacancies in resistivity with increasing the substrate temperature can be
have lower formation energy than the zinc interstitial, they attributed to the desorption of oxygen from the surface at
should be more abundant. The redshift and increase in the higher substrate temperature and thus increase in the concen-
intensity of the photoluminescence are likely to be due to the tration of the oxygen vacancies. The increase in resistivity on
desorption of oxygen from the film surface at higher sub- annealing the film in oxygen ambient can be attributed to the
strate temperature. It causes the formation of oxygen vacan- absorption of oxygen and thus reducing the concentration of
cies and removal of other defects states such as antisite Zn oxygen vacancies and interstitial zinc, which reduced the
and oxygen in the film. Figure 2共b兲 shows the PL spectra of concentration of free carrier produced by zinc interstitial and
as-deposited and annealed ZnO films on Si. In as-deposited oxygen vacancies from the film.
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6
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