Thin Solid Films 476 (2005) 59 64

www.elsevier.com/locate/tsf

A statistical parameter study of indium tin oxide thin films

deposited by radio-frequency sputtering
Seung-Ik Juna,*, Timothy E. McKnightb, Michael L. Simpsona,b, Philip D. Racka
b

a
Department of Materials Science and Engineering, The University of Tennessee, Knoxville, TN 37996, USA
Molecular Scale Engineering and Nanoscale Technologies Research Group, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA

Received 31 May 2004; received in revised form 18 August 2004; accepted 2 September 2004
Available online 30 October 2004

Abstract
In order to optimize the electrical and optical properties of indium tin oxide (ITO) thin films, a statistical analysis called Taguchi design
was employed. It is shown that the sheet resistance and transmittance are inversely proportional to each other as a function of the process
parameters. Additionally, the preferred orientation of crystalline ITO film is distinguishably changed with the increase of sputtering
temperature and oxygen fraction (O2/O2+Ar) in the sputtering ambient. The change in crystallinity results from the content of incorporated
oxygen, which significantly affects the electrical and optical properties of ITO films and causes a rearrangement of atoms to form preferred
closed-packed plane orientation. Finally, the microstructure of the ITO films becomes denser with the increasing oxygen fraction. As a result
of this work, we have successfully achieved low sheet resistance (7.0 V/5) and high transmittance (~90%) for 300 nm thick films.
D 2004 Elsevier B.V. All rights reserved.
PACS: 73.50.-h; 78.20.-e
Keywords: Indium tin oxide (ITO); Sputtering; Taguchi design; Transparent electrode

1. Introduction
Indium tin oxide (ITO) thin films are widely used as
transparent electrodes in electronic displays [1]. In recent
years, ITO has also been implemented in light-addressed
intracellular biological probes [2,3]. Normally RF magnetron sputtering is used for the deposition of the film because
it provides a low temperature deposition process and higher
process efficiencies, higher throughput, and process reliability [1]. When using ITO transparent electrodes, there is a
well-known trade-off between the sheet resistance and the
transmittance, which is dominated by the number of oxygen
vacancies in the films [4,5]. Oxygen vacancies are donor
levels in ITO; consequently, when ITO is slightly oxygendeficient, reasonable electrical transport can be realized. The
transmittance however can be deleteriously affected if the

* Corresponding author. Tel./fax: +1 865 974 0033.

E-mail address: sjun3@utk.edu (S.-I. Jun).
0040-6090/$ - see front matter D 2004 Elsevier B.V. All rights reserved.
doi:10.1016/j.tsf.2004.09.011

films are too oxygen-deficient as they become more metallike. Therefore it is important to determine the optimized
deposition conditions in order to achieve high transmittance
and low sheet resistance at the same time. In a typical RF
magnetron sputtering system, normally there are four main
factors that control the process; RF power, gas pressure,
temperature, and gas composition. To optimize this wide
parameter space in a serial manner is tedious and unwieldy
and many parameter interactions can go undetected. To
facilitate rapid process optimization and reduce the number
of trials and analytical errors, statistical tools can be
implemented. In this research, we describe a Taguchi design
of experiment (DOE) for the purpose of optimizing the ITO
deposition [6,7]. This DOE is normally used for optimizing
a process condition that is completely unknown or in the
initial stage of process development to determine the overall
tendencies of process factors with less experiment trials [7].
The process targets for the ITO films are sheet resistance
b10 V/5 and transmittance (at 488 nm) N85% for a nominal
film thickness of 300 nm.

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S.-I. Jun et al. / Thin Solid Films 476 (2005) 5964

2. Experimental details
The specified description of the DOE is described in
detail in Table 1. Our initial DOE was a three-level
design (low, medium, high) for the four process factors,
which included RF power, temperature, pressure, and O2
fraction (for a Ar+O2 ambient). The responses for the
DOE included deposition rate, transmittance, sheet resistance, and etching rate. For the DOE analysis, a high
deposition rate, high transmittance, low sheet resistance,
and high etch rate were desirable. Consequently, to
qualify how the factors affected our responses, the
following illustrates our interpretation of the results:
dlarger is betterT for deposition rate, dlarger is bestT for
transmittance, dsmaller is bestT for sheet resistance, and
dlarger is betterT for etching rate.
An AJA ATC2000 RF magnetron sputtering system
was utilized for the deposition of ITO thin films on glass
substrates. The sputtering target has a diameter of 50 mm
and a thickness of 6 mm and consists of In2O3 and 10
wt.% SnO2. The base pressure prior to the sputtering
deposition was below 5.310 6 Pa and the total flow rate
of argon used in the sputtering was fixed at 25 sccm for
all conditions. The substrate is heated by quartz lamps
and the temperature is controlled within F1 8C.
The transmittance of ITO thin films was measured
using a calibrated Ar lamp and an Ocean Optics PC2000
spectrometer with a wavelength range 200900 nm. The
transmittance was fixed and normalized at 488 nm
because our application is a light-addressed biological
probe operated at that wavelength because silicon is the
active layer and has a high absorption coefficient at 488
nm. The sheet resistance was analyzed via four-point
probes (Veeco FPP-5000) and the reported value is an
average of three measurements over the sample. The film
thickness and etching rate were evaluated by using
Surface Profiler (KLA Tencor Alpha-Step 500). The

Fig. 1. Effects of RF power, temperature, pressure, and gas composition on

the deposition rate, sheet resistance, and transmittance.

etchant was a solution of HCl+CH3COOH+H2O (22%+

6%+72%) and heated and maintained at 40 8C on a hot
plate. The crystal orientation of ITO thin films was
determined by a Phillips X-pert Pro X-ray diffraction

Table 1
DOE for optimizing ITO thin film deposited by RF magnetron sputtering: Taguchi design
No.

Factors

1
2
3
4
5
6
7
8
9
a
b
c
d

Responses

RF power,
W (W/cm2)

Temperature,
8C

Pressure,
Pa

O2 ,
sccm

D/Ra,
nm/min

Trb,
%

Rsc,
V/5

E/Rd,
nm/min

75
75
75
100
100
100
125
125
125

30
130
230
30
130
230
30
130
230

0.7
2.0
3.3
2.0
3.3
0.7
3.3
0.7
2.0

0
2
4
4
0
2
2
4
0

2.63
0.67
0.14
0.82
0.93
2.91
0.84
3.43
2.52

35.1
86.1
89.5
87.2
85.8
88.9
89.2
86.8
68.6

262
63,593
391
~150,000
231
343
~150,000
10,839
28

N200
N200
b5
N200
N200
424
N2000
545
403

(3.7)
(3.7)
(3.7)
(4.9)
(4.9)
(4.9)
(6.2)
(6.2)
(6.2)

D/R: deposition rate (nm/min).

Tr: transmittance at 488 nm (%).
Rs: sheet resistance (V/5) at 300 nm thickness films.
E/R: etching rate in HCl+CH3COOH+H2O (22%+6%+72%), 40 8C.

S.-I. Jun et al. / Thin Solid Films 476 (2005) 5964

Table 2
Optimum levels for each factor and its priority in optimizing ITO deposition
Targets

RF power

Temperature

Pressure

O2 content

Lower Rs
Higher Tr
Higher D/R
Optimized

Low
High
High (2)
Low
(b75 W)

High (1)
High
High
High
(N230 8C)

Low
High (2)
Low (1)
Low
(b0.7 Pa)

Low (2)
High (1)
Low
Low
(~0 sccm)

(1), (2): The first and second priorities effecting on process targets.

(XRD) and the microstructure was evaluated using a

Hitachi S-4300 scanning electron microscope (SEM).

3. Results and discussion

The DOE used in this work and its results are illustrated
in Table 1. As previously mentioned, the process factors
are RF power, temperature, gas pressure, and oxygen
fraction. The effects of the process factors on the
deposition rate, sheet resistance, and transmittance at 488
nm, and etching rate following experiments are presented
in Table 1 and tendencies are illustrated in Fig. 1. As
shown in Fig. 1, the main factors that strongly effect on
the deposition rate are pressure and RF power, with total
pressure having the strongest effect. The significant lowering of the deposition rate with increasing pressure is a
result of the shorter mean free path of the sputtered species
as the pressure is increased. As pressure increases, the
sputtered species get scattered while traversing the ~130
mm target-to-substrate distance. According to the kinetic
theory of gas, the thermal mean free paths at 0.7, 2.0, and
3.3 Pa are ~54, 18, and 11 mm, respectively. Another
interesting observation from Fig. 1 is that the deposition
rate decreases with increasing oxygen flow. We also
surveyed XRD results and concluded that the deposition
rate was lowered by oxygen addition due to the change
from amorphous to crystalline ITO and the transformation

61

of its preferred crystallinity [8]. A detailed explanation of

this phenomenon will be discussed later.
Fig. 1 also shows the effects that the four factors have on
sheet resistance and illustrates that temperature is the most
dominant factor affecting the sheet resistance of the ITO
films. As the temperature is increased, the sheet resistance
can be lowered significantly. The reason for the observed
decrease in the sheet resistance with increasing temperature
is a structural amorphous-to-crystalline transformation in the
ITO films as will be discussed in detail below. The observed
relationship of decreasing sheet resistance with decreasing
RF power can also be correlated to the crystallinity of the
ITO films as determined from the XRD data [9].
The effect that the four factors have on the transmittance
of ITO films is one of the critical responses of the DOE and
the prevailing factor is the flow rate of oxygen. In the
process of Ar sputtering (no oxygen), the oxygen concentration of the ITO film is lower than that of the target
because not all the oxygen sputtered from the target will be
incorporated into the film. That is, the films without oxygen
flow show metal-like characteristics with low transmittance,
low sheet resistance, and higher oxygen vacancy concentration. On the other hand, as the oxygen fraction is
increased in sputtering gas, the concentration of oxygen
vacancies is drastically decreased and it results in higher
transmittance and higher sheet resistance like an oxide
insulating thin film [10,11].
The optimum levels of each factor and its priority are
summarized in Table 2. Optimized levels from the Taguchi
DOE are lower RF power, higher temperature, lower
pressure, and lower oxygen contents in order to minimize
sheet resistance and to maximize transmittance of ITO films
at the same time.
In order to optimize the dominant factors of temperature
and oxygen fraction, a second experiment was designed as
shown in Table 3. For this experiment, the total pressure and
Ar flow rate were fixed at 0.7 Pa and 25 sccm, respectively,
for all conditions. Finally, we compared the optimized

Table 3
Additional experiment for optimizing dominant factors: temperature and O2/(O2+Ar) ratio
No.

1
2
3
4
5
6
7
8
9b

Factors

Responses

RF power,
W (W/cm2)

Temperature,
8C

O2/(O2+Ar)

D/R,
nm/min

Tr,
%

Rs,
V/5

XRD
intensitya

75
75
75
75
75
75
125
125
125

400
400
400
400
400
400
400
30
30

0.00
0.01
0.02
0.04
0.06
0.08
0.00
0.00
0.00

3.23
3.29
3.19
2.81
2.56
2.39
4.70
3.22
3.22

87.3
82.7
81.5
92.8
98.1
96.6
68.2
75.8
85.9

7.0
97.2
242.1
201.5
339.8
479.3
8.9
206.0
8.2

405
305
295
334
804
954
440
164
369

(3.7)
(3.7)
(3.7)
(3.7)
(3.7)
(3.7)
(6.2)
(6.2)
(6.2)

All films are deposited at 0.7 Pa pressure.

a
(222) intensity.
b
Post-annealed after room temperature deposition (400 8C, 30 min in the vacuum).

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S.-I. Jun et al. / Thin Solid Films 476 (2005) 5964

Fig. 2. XRD pattern for sintered ITO target containing In2O3 and 10 wt.%
SnO2.

Fig. 4. XRD patterns for two different applied RF powers.

condition from the DOE with a film deposited at room

temperature and post-annealed at 400 8C, 30 min (experiment no. 9).
Fig. 2 shows that XRD pattern of a sintered ITO
sputtering target, which shows that the preferred orientation
is (222). Additionally, the other dominant orientations in
this pattern are (211), (400), (440), and (622).
The XRD patterns of the ITO films at different substrate
temperature are shown in Fig. 3. All were done under 0.7 Pa
of pressure, 75 W (3.7 W/cm2) of RF power, and 25 sccm of
Ar flow rate. From Fig. 3, it is seen that the crystallinity of
the ITO film deposited at room temperature is almost
amorphous ITO. However, as the substrate temperature is
increased during deposition, the crystallinity increases with
(400) preferred orientation mixed with small amounts of
(222), (440), and (620). These results are similar to those
observed in the initial DOE. The reason for (400) preferred
orientation is that the concentration of oxygen vacancies in
the ITO film at high temperature sputtering is higher than
that of room temperature sputtering because of the reduced
sticking coefficient of oxygen at higher temperatures.
Therefore crystalline ITO deposited high temperature
typically grows (400) preferentially to accommodate the
oxygen vacancies on these planes. On the other hand, the
post-annealed ITO film at 400 8C/30 min that was deposited
at room temperature shows (222) preferred plane that is a
close-packed plane in In2O3 body-centered cubic structure.

This plane does not accommodate vacancies very well and

is stabilized when there are fewer oxygen vacancies.
Fig. 4 shows the dependence of the RF power on the
XRD patterns. Both are processed under 0.7 Pa of
pressure, 400 8C of temperature, and 25 sccm of argon
flow rate (without oxygen). The slight increase of intensity
explains that the increase of RF power results in wellcrystallized structure due to the impinging of higher energy
ions onto substrate.
Fig. 5 shows the XRD results according to the fraction of
oxygen in sputtering gas. The sputtering conditions were 0.7
Pa, RF power of 75 W (3.7 W/cm2), 25 sccm of argon flow
rate, and substrate temperature of 400 8C. In argon alone,
there are two dominant planes in the film, (222) and (400).
As the fraction of oxygen is increased, the (400) peak
disappears and (222) peak becomes the dominant plane. We
can speculate from these results that the driving forces of
this change in preferred orientation are the concentration of
oxygen vacancies and their subsequent diffusion. If the
deposition is processed with zero or low oxygen, more
oxygen vacancies are incorporated in the ITO film versus
those films processed at higher oxygen fractions in the
sputtering gas. The vacancies play an important role in
atomic diffusion and the atoms can diffuse through these
vacancies. Therefore we can infer that various preferred
planes are shown in argon sputtering without oxygen. On

Fig. 3. XRD results according to substrate temperature and post-annealing.

Fig. 5. XRD results as a function of fraction of oxygen in sputtering gas.

S.-I. Jun et al. / Thin Solid Films 476 (2005) 5964

63

the other hand, as the fraction of oxygen is increased, the

concentration of oxygen vacancies is decreased. As a result,
the (222) peak will dominate in higher oxygen content in the
sputtering ambient since the close-packed plane is (222) in
the body-centered cubic In2O3 crystal.
The relationship between transmittance and sheet
resistance is illustrated in Fig. 6. All were deposited at
0.7 Pa pressure, 400 8C temperature, and 75 W RF power.
The trend done in the first DOE is observed in the second
experiment: namely, the transmittance and sheet resistance
both have increasing relationship as the fraction of oxygen
is increased. Specifically, the transmittance decreases when
the sheet resistance is lowered. As the fraction of oxygen
increased, the incorporated oxygen in the film will
contribute to the enhancement of transmittance but the
sheet resistance will be increased and deteriorated by the
oxygen contrariwise. It results from the incorporated
oxygen which decreases the donor level concentration
and increases the sheet resistance and concomitantly
increases the transmittance.
It was previously concluded from original DOE that this
results from the formation of oxygen vacancies in the film
when it is deposited in argon gas only. In Fig. 6, we also can
see that the deposition rate is lowered by addition of oxygen
gas because the preferred plane of the film is clearly
changed from the (400) plane that is perpendicular to
substrate into (222) plane with the increase of oxygen
fraction in gas. In lower oxygen ambient, the ITO film was
grown as (400) preferentially with higher oxygen vacancies

Fig. 7. SEM image of ITO film with the increase of oxygen in gas: (a) O2/
(O2+Ar): 0.00; (b) 0.02; (c) 0.08.

and higher deposition rate. On the other hand, in higher

oxygen gas, the film was arranged to (222) plane that is
most close-packed plane in In2O3 having a BCC structure.
Therefore the deposition rate decreases with the increase of
oxygen addition in plasma because the (222) close-packed
plane is denser than the (400) plane which accommodates
more vacancies.
Fig. 7 shows the SEM images as the oxygen fraction is
increased from 0.00 to 0.08. This result shows that the ITO
grains become coarser and denser with the increase of
oxygen.

4. Conclusions

Fig. 6. The characteristics of transmittance, sheet resistance, deposition rate,

and XRD intensity (222) as a function of oxygen fraction in sputtering.

To improve the electrical properties, lower sheet resistance, ITO deposition should be processed under higher
temperature and low oxygen fraction. A tradeoff between

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S.-I. Jun et al. / Thin Solid Films 476 (2005) 5964

low sheet resistance and high transmission exists due to the

role that the oxygen vacancies have in the conduction and
transmission. A high number of oxygen vacancies facilitate
conduction; however, the film becomes less transparent.
Conversely, few vacancies facilitate high transmission;
however, the conduction decreases significantly. To rapidly
determine an optimum process for ITO films, a Taguchi
design of experiments was implemented to investigate the
effects that RF power, substrate temperature, total pressure,
and oxygen partial pressure have on the sheet resistance,
transmission, deposition rate, and etch rate. The effects that
each process parameter had on each response were shown.
The oxygen partial pressure was determined to be the
dominant factor that controlled the sheet resistance and
transmission so a subsequent experimental design was run to
closely determine the effect of oxygen partial pressure on the
ITO films. The properties were correlated to the crystal
structure and microstructure of the ITO films. It was
discovered that the optical and electrical properties are
strongly correlated to the preferred orientation of the films
which varies from (400) to (222) as the fraction of oxygen in
sputtering increases. We speculate that the preferred orientation is a result of the concentration of oxygen vacancy
and rearrangement of atoms in close-packed plane of In2O3
having a body-centered cubic structure. As shown in the
above results, the crystallinity of ITO films strongly depends
on temperature, RF power, and oxygen fraction in sputtering.
Specifically, high temperature, energetic ion bombardment
due to higher RF power, and less oxygen vacancy due to
addition of oxygen gas in sputtering ambient all contribute to
the enhancement of the crystallinity of the films.

Acknowledgements
This work was supported in part by the National Institute
for Biomedical Imaging and Bioengineering under assignment R01EB000433 and through the Laboratory Directed
Research and Development funding program of the Oak
Ridge National Laboratory, which is managed for the U.S.
Department of Energy by UT-Battelle, LLC.

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