Design of Low Surface Roughness-Low Residual Stress-High Optoelectronic Merit a-IZO Thin Films For Flexible OLEDs

Design of low surface roughness-low residual stress-high
optoelectronic merit a-IZO thin films for flexible OLEDs

Naveen Kumar,1 Taylor M. Wilkinson,2 Corinne E. Packard,2* Mukesh Kumar1*
1
Functional and Renewable Energy Materials Laboratory, Indian Institute of Technology Ropar, Punjab-
140001, INDIA
2
Metallurgical and Materials Engineering, Colorado School of Mines, Golden, CO, USA
Abstract
The development of efficient and reliable large-area flexible optoelectronic devices demands
low surface roughness-low residual stress-high optoelectronic merit transparent conducting
oxide (TCO) thin films. Here, we correlate surface roughness-residual stress-optoelectronic
properties of sputtered amorphous indium zinc oxide (a-IZO) thin films using a statistical
design of experiment (DOE) approach and find a common growth space to achieve a smooth
surface in a stress-free and high optoelectronic merit a-IZO thin film. The sputtering power,
growth pressure, oxygen partial pressure and RF/(RF+DC) are varied in a two-level system
with a full factorial design, and results are used to deconvolve the complex growth space,
identifying significant control growth parameters and their possible interactions. The surface
roughness of a-IZO thin film varies over 0.19 nm to 3.97 nm, which is not in line with the
general assumption of low surface roughness in a-IZO thin films. The initial regression model
and analysis of variance reveal no single optimum growth sub-space to achieve low surface
roughness (≤0.5 nm), low residual stress (-1 to 0 GPa) and industrially acceptable electrical
conductivity (>1000 S/cm) for a-IZO thin films. The extrapolation of growth parameters in
light of the current results and previous knowledge leads to a new sub-space, resulting in a
low residual stress of -0.52±0.04 GPa, a low surface roughness of 0.55±0.03 nm and
moderate electrical conductivity of 1962±3.84 S/cm in a-IZO thin films. These results
demonstrate the utility of the DOE approach to multi-parameter optimization, which provides
an important tool for the development of flexible TCOs for next-generation flexible OLED
applications.
Keywords: amorphous indium zinc oxide, surface roughness, residual stress, design of
experiments (DOE), analysis of variance(ANOVA) and organic light emitting diode (OLED)
___________________________________________________________________________
Corresponding author: mkumar@iitrpr.ac.in and cpackard@mines.edu
Pursuant to the DOE Public Access Plan, this document represents the authors' peer-reviewed, accepted manuscript.
The published version of the article is available from the relevant publisher.
I. INTRODUCTION
Transparent conducting oxides (TCO) with high electrical conductivity (103 S/cm)
and wide optical transparency (>80% in 300-1100 nm range) have potential applications in
numerous displays, solar cells and electrochromic devices [1-4]. Recently, organic light
emitting diodes (OLED) have received impressive scientific and technological interest driven
by their potential usage in a large variety of display technologies [5, 6]. OLEDs are fabricated
on TCO electrodes that also work as an anode in the layered structure of TCO/hole transport
layer/emitter layer/electron transport layer/metal electrode and help to inject the holes carriers
from hole transport layers into emitter layers[1]. Therefore, the morphology of TCO thin
films and interface quality between TCO anode and the hole transport layer critically impacts
the charge injection and luminescence quantum efficiency in OLEDs [5, 7, 8]. The surface
roughness of TCO electrodes was observed to critically impact the performance in term of
long time reliability. Tin-doped indium oxide (ITO) is considered as an industrial standard
TCO material because of its good optoelectronic properties, making it suitable for
photovoltaics and OLEDs displays applications. On the other hand, the high surface
roughness of stable crystalline ITO thin films results in fast degradation and dark spots in
OLEDs [9, 10]. Amorphous ITO films, which can have low surface roughness, are observed
to be unstable and transform to a polycrystalline phase with time and exposure to humid
environments can further increase roughness, causing time-dependent degradation of
performance [11]. Tak et al. have reported the performance of OLEDs with ITO electrodes
having surface roughness (peak-to-valley, Rpv) in the range of 8-16 nm and observed high
linkage current that increased with surface roughness [9]. In another report, Jonda and co-
workers observed the effect of surface roughness on the degradation of OLEDs [12]. A root
mean square surface roughness of 2.7 nm and peak-to-valley variation of 21 nm were
observed for ITO thin films; inhomogeneity in the emitter layer and hot spots leading to fast
degrades OLEDs were attributed to the roughness. Yang et al. has fabricated OLED on glass
and PET substrates with ion assisted deposition (IAD) to reduce growth temperature, and to
improve adhesion and morphology of the ITO layer for better performance. Improved
electroluminescence performance was reported for ITO coated glass substrates, which had
nearly 1 nm (RMS) surface roughness for the ITO deposited on glass, compared to 3.6 nm
over the same area for ITO films deposited on PET [5].There are many other reports of
coating polymers on top of ITO to make it smoother. In this case, the sacrificial polymer
layer should match hole injection levels between ITO and hole transport layers of OLEDs,
which make the material choice complex. In flexible OLEDs applications, TCOs must
withstand repeated flexing without losing physical or electrical contact with the bottom
flexible substrate and top hole transport layer, and throughout the film. Industry standard
ITO thin films show crack propagation over bending that may degrade flexible OLED with
time [13, 14]. Furthermore, the requirement of high deposition temperatures (>300°C) for
favourable optoelectronic properties and high residual stress in crystalline ITO thin films
impedes their usage for next generation flexible OLED applications [15-19].Therefore, it has
become necessary to develop alternative TCO thin films to replace ITO anode electrodes.
Amorphous indium zinc oxide (a-IZO) with a metal composition in the range of 55–84
cation% indium is a thermally stable, amorphous TCO with a crystallization temperature
(600C) much higher than standard ITO thin films [20]. IZO thin films have been grown at
nearly room temperature with a conductivity of ∼3000 S/cm, high electron mobility in the
range of 10–50 cm2/V and high transmittance of >90% in visible to NIR region [20, 21]. W.
J. Lee et al. has fabricated OLED on IZO of roughness ~0.7 nm, showing better
electroluminescence performance than OLEDs fabricated on a commercial ITO anode [22].
Recently, Kim and co-workers reported stable bending performance of flexible OLEDs using
IZO thin film as an anode [23]. Based on the figure-of-merit ( Φ = Tq/Rs, transmittance is
measured at 550 nm ), IZO was observed to be a superior anode electrode for next generation
flexible OLEDs in comparison to a metal nanowire network, conducting polymers and other
hybrid electrodes [1]. Although, a-IZO showed a smooth surface with surface roughness, <
1nm [20] (which is much less than crystalline ITO), variation in surface roughness from 0.49
nm to 0.89 nm in a-IZO was reported to affect the turn-on voltage and luminescence
properties of OLEDs [24]. In our previous report, we have demonstrated that a-IZO thin films
with optimum optoelectronic properties have high amounts of compressive residual stress
that could cause unintentional bending and impede stacking of various layers during
assembly of the flexible OLEDs [25]. Therefore, structural optimization should be
considered, together with residual stress and optoelectronic properties, for high performance,
long term reliability and mechanically robust flexible OLED devices.
In this work, surface roughness, residual stress, and optoelectronic properties of a-IZO thin
films were optimized for next generation flexible OLED applications. The surface roughness
(rms values) of room temperature grown a-IZO thin films were observed to vary from
0.19±0.04 nm to 3.97±1.28 nm. High residual stress in the range of +1.68±0.51 GPa (tensile
residual stress) to -4.36±0.49 GPa (compressive residual stress) was observed for the same
set of a-IZO thin films grown, as reported in a previous study [25]. Moderate optoelectronic
properties were observed, includingelectrical conductivity 2520 S/cm and visible
transmission of 90%, for highly compressive stressed a-IZO thin films. Therefore, to
achieve low surface roughness, low residual stress and high optoelectronic merits,
understanding the complex growth space and interdependencies of growth parameters in the
sputtering deposition process is required. We revisited the design of experiment approach and
searched a new growth space for the simultaneous optimization of structural-mechanical-
optoelectronic properties of a-IZO thin films. Since higher surface roughness in a-IZO was
reported to affect the turn-on voltage and luminescence properties of OLEDs [5, 7], the target
surface roughness in the present study is set 0.5 nm of less. By extrapolating the growth
space, we successfully achieved a smooth a-IZO thin film with surface roughness of
0.55±0.03nm, low residual stress of -0.52±0.04 GPa and a moderate electrical conductivity of
1962.22 ± 3.84 S/cm.
II. EXPERIMENTAL DETAILS
The details of a-IZO thin film fabrication are given elsewhere [25]. In brief, IZO thin
films were fabricated by using DC/RF sputtering technique from a 99.999% pure IZO target
(In2O3/ZnO: 87/13 wt % Materion Inc.). For the precise control and measurement of low
oxygen partial pressure during the growth of IZO thin films, a residual gas analyser (RGA)
with a partial differential pump was used. To access a wide sputtering growth space and to
optimize IZO thin films for low roughness, low residual stress and high optoelectronic
properties, the growth parameters of sputtering power (Pw), growth pressure (Pr), Oxygen
partial pressure (PO2) and RF/DC power ratio, RF/(RF+DC), were selected for variation.
The lower and upper limits of Pr, PO2, and RF/(RF+DC) were selected to encompass a wide
range of stable sputtering conditions reported in literature and possible in the current
deposition system. The power was selected to vary from 25 W to 150 W while the oxygen
partial pressure was varied from 1 to 3%. The growth pressure was selected to vary from 4
mtorr to 10 mtorr while the power ratio was varied from pure DC to pure RF. Two levels, low
and high, were chosen for each growth parameter to encompass a wide range of combinations
of sputtering conditions. A center point between the low and high level was also chosen to
check linearity assumptions between low and high values of growth parameters [25].
Therefore, LevelFactor +center point: 24+1=17 was the total number of experiments, performed
with different combinations of sputtering growth parameters. The electrical conductivity and
residual stress of as-grown a-IZO thin films were measured by using Hall effect
measurements and cantilever deflection techniques, respectively, which were discussed in
detail elsewhere [25]. The surface roughness of a-IZO thin films was characterized using a
Bruker scanning probe microscope in tapping mode. We used an RTESP model tip having a
spring constant and resonance frequency of 40 N/m and 300 kHz, respectively. The
roughness measurement was done at five different sites on each IZO thin film sample with a
scan area of 1µm×1µm. The root mean square roughnesses of the a-IZO thin films were then
averaged out over the five different areas per sample. The residual stress of the films was
measured by the cantilever deflection method [25]. In this technique, a IZO thin film was
deposited on flexible glass substrate, with thickness of 140-150 µm, and deflection due to the
residual stress in the thin films was measured with respect to a flat Si reference.
Table 1: The measured residual stress, electrical conductivity and surface roughness on full
factorial design for IZO thin film samples with two levels and four growth parameters
[sputtering power P, growth pressure Pr, Oxygen partial pressure PO2and RF ratio
RF/(RF+DC)] and one center point.
S. Growth parameters Residual Electrical Surface

No stress (GPa)* conductivity roughness
P (W) Pr PO2(%) RF/(RF+DC) (S/cm)* (nm)
(mtorr)
1 25 4 1 0 -4.36±0.49 1921 ± 0.2 0.19 ± 0.04
2 150 4 1 0 -2.25±0.3 2479 ± 0.35 0.96 ± 0.04
3 25 10 1 0 -0.37±0.08 1.44 ± 0.01 1.14 ± 0.13
4 150 10 1 0 -2.33±0.38 2520 ± 0.02 2.38 ± 0.76
5 25 4 3 0 -3.32±0.4 2150 ± 0.15 0.27 ± 0.06
6 150 4 3 0 -3.27±0.59 2280 ± 0.02 0.22 ± 0.03
7 25 10 3 0 -0.71±0.38 0.06 ± 0.002 1.02 ± 0.27
8 150 10 3 0 -2.56±0.3 1970 ± 0.05 3.97± 1.28
9 25 4 1 1 -0.79±0.1 28.2 ± 0.01 0.95 ± 0.09
10 150 4 1 1 -2.82±0.72 1780 ± 0.7 0.26± 0.02
11 25 10 1 1 1.68±0.51 0.87 ± 0.001 0.83 ± 0.07
12 150 10 1 1 -2.63±0.33 1744 ± 0.35 1.92 ± 0.13
13 25 4 3 1 -1.81±0.43 6.64 ± 0.002 2.54± 0.45
14 150 4 3 1 -2.91±0.4 375 ± 0.1 1.16 ± 0.27
15 25 10 3 1 -2.52±0.7 0.082 ± 0.001 0.48 ± 0.15
16 150 10 3 1 -1.56±0.35 12.1 ± 0.002 0.35 ± 0.02
17 87.5 7 2 0.5 -2.74±0.5 2430 ± 0.002 0.37 ± 0.06
*Residual stress and electrical conductivity data are reproduced from Ref.[25]
A comprehensive list of measured surface roughness, residual stress and optoelectronic
properties along with their corresponding growth parameters is listed in table 1. The data for
residual stress and electrical conductivity from our previous study is reproduced here for ease
of reference [25]. To understand the interdependencies of growth parameters for surface
roughness, residual stress and electrical conductivity, Minitab-17 statistical software was
used.
III. RESULTS AND DISCUSSION
In the previous study, we achieved low residual stress and moderate electrical
conductivity by exploring the growth space in the region of low oxygen partial pressure of
0.5%, low sputtering powers of 35 W and 50 W, middle RF/DC ratio of 0.5 and high
deposition pressure of 9 mtorr. Two growth conditions were proposed to simultaneously
achieve low residual stress and the moderate electrical conductivity (sample A: P = 35 W, Pr
= 9 mtorr, PO2 = 0.5% and RF/(RF+DC) = 0.5 and sample B: P = 35 W, Pr = 9 mtorr, PO2 =
0.5% and RF/(RF+DC) = 0.5). To explore whether a-IZO thin films optimized for low
residual stress and moderate electrical conductivity have sufficiently low surface roughness
for OLED applications (≤0.5 nm), we performed AFM on the previously optimized films.
The surface topography is shown for sample-A and sample-B in Figures 1(a) and 1(b),
respectively.
(a) (b)
FIG. 1. Atomic force microscopy images (1×1 µm2) of a-IZO thin films deposited on glass
substrates using sputtering powers of (a) 35 W and (b) 50 W. The growth pressure, oxygen
partial pressure and RF/DC ratio of 9 mtorr, 0.5 % and 0.5, respectively were common
growth parameters for both the films. Both films exhibit roughness in excess of 1 nm.
The roughnesses of the optimized sample-A and sample-B are 1.25±0.16 nm and 1.93±0.14
nm, respectively. It is clear that these a-IZO thin films have surface roughnesses too large for
use in OLEDs, despite possessing low residual stress and moderate electrical conductivity. To
simultaneously optimize a-IZO thin films for low surface roughness, low residual stress and
moderate electrical conductivity, we measured surface roughness of all the thin films listed in
Table 1. The measured surface topography of a-IZO thin film samples is shown in Figure 2.
The number in each image is the same as the serial number mentioned in Table 1. We have
excluded the image corresponding to the center point, sample #17, to maintain the symmetry
in the Figure 2. The measured surface roughness of a-IZO films was found to vary from
0.19±0.04 nm to 3.97±1.28 nm over the series. Lowest and highest surface roughnesses of
0.19±0.04 nm and 3.97±1.28 nm, respectively, were found for growth conditions of P=25W,
Pr=4mtorr, PO2=1%, RF/(RF+DC)=0 and P=150W, Pr=10mtorr, PO2=3%, RF/(RF+DC)=0,
respectively.
FIG.2. Atomic force microscopy images (1×1 µm2) of a-IZO thin films deposited on glass
substrates using growth conditions in Table 1, using the same sample numbering scheme.
From the data in Table 1, it is clear that the IZO thin film with the lowest surface roughness
of 0.19±0.04 nm has the highest compressive residual stress of 4.36±0.49 GPa and moderate
electrical conductivity of 1921±0.2 S/cm, while the IZO thin film with the highest surface
roughness has moderate compressive residual stress of 2.56±0.3 GPa and moderate electrical
conductivity of 1970±0.05 S/cm. Therefore, there is no direct correlation among surface
roughness, residual stress and electrical conductivity of a-IZO thin films. To shed some light,
we plotted all the data of surface roughness vs. residual stress and surface roughness vs.
electrical conductivity from Table 1, independent of their growth parameters. The results are
shown in Figures 3(a) and 3(b). The data points are labelled according to Table 1.
(a) (b)
FIG.3. (a) Residual stress vs. surface roughnessand (b) Electrical conductivity vs. surface
roughness of IZO thin films. Shaded area perpendicular to x-axis and y-axis denotes desire
surface roughness (0.5nm) and residual stress (0 to -1 GPa) and electrical conductivty
(>1000 S/cm) in (a) and (b). The common green area indicates target regions for residual
stress, surface roughness and electrical conductivity.
The green box region of the two intersections in Figures 3(a) and 3(b) shows the common
target area of low surface roughness (≤0.5 nm) with low residual stress (0 to -1 GPa) and
acceptable moderate electrical conductivity (>1000 S/cm), respectively. Figure 3(a) shows
the surface roughness vs residual stress for a-IZO thin films. No initial growth conditions
fulfill both the roughness and residual stress criteria. Figure 3(b) shows data from the same
samples, now with the surface rougness vs. electrical conductivity plotted for a-IZO thin
films listed in Table 1. There are five growth conditions, #1, 5, 6, 10 and 17, that fulfill both
roughness and electrical conducitibity criteria. The a-IZO thin film with low surface
roughness (<0.5 nm ) and moderate electrical conductivity (>1000 S/cm) shows high residual
stress (-2.82 GPa to -4.36 GPa). Therefore, there is no single growth condition in the intial
growth space that satisfies the requirement for a-IZO with low surface roughness, low
residual stress and simultaneously high electrical conductivity. This motivated us to complete
additional optimization of a-IZO thin films.
To understand the impact of growth parameters on surface roughness, electrical conductivity

and residual stress of a-IZO thin films, we explored sputtering phenomenon indepth. These
properties are widely affected by sputtering growth parameters like sputtering power,
sputtering pressure, oxygen partial pressure and RF/DC ratio. The most significant conditions
affecting the residual stress, electrical conductivity and surface roughness are the energy of
ions and neutral atoms sticking on growing film surfaces and the ionization efficiency of
neutral atoms in the plasma [26]. More than one growth parameter affects these properties. It
was reported that the maximum energy for singlely charged oxygen ions was found to be 70
eV near the growing film surface at 6 mtorr of growth pressure [27]. This energy critically
affected the residual stress even in amorphous thin films [25]. Ito et al. reported that residual
stress of aluminium doped zinc oxide films changes from compressive to tensile with increse
in RF/DC ratio due to change in ionization efficiency of different species in the plasma [28].
In amorphous thin films, compressive and tensile residual stresses may arise due to the
bombardment of energetic ions which result in changes in material density at the film’s
surface, called the atomic peening effect [29]. The energy of different ionic and neutral
species in the plasma during the sputtering process critically depends on sputtering power,
growth pressure, oxygen partial pressure and RF/DC ratio and affect the residual stress in a-
IZO thin films.
Morever, the electrical conductivity of IZO thin films can be increased by either increasing
carrier concentration or carrier mobility. Moreover, in a-IZO thin films the overlapping of
post transition metal’s ns orbitals gives the path for conduction of electrons and makes the
material less prone to structural disorder [30, 31]. In our previous work, it was observed that
the electrical conductivity increases with sputtering power and decreases with growth
pressure [25]. On the other hand, surface roughness which directly corelates to the surface
topography, is affected by several growth parameters which we have already mentioned
above. At high growth pressure, sputtered ions have low energy due to frequent collisions
among neutral atom and leads to low mobility of adatoms which limits the coalescence and
forms smaller grains; just the opposite effect was reported for low/moderate sputtering
pressure. Higher mobility of adatoms results in a rougher surface [32]. Jung and co workers
have explained that the roughness of tin-doped indium oxide (ITO) depends on adatom
mobility which is a function of sputtering pressure, sputtering power and substrate
temperature [32]. Carcia et al. also showed that the increase in surface rougness with an
increase in oxygen partial pressure of ITO deposited on PET increases due to negative ion
bombardment on the growing thin film [27]. J. B. Park and co-workers reported the effect of
RF/DC ratio on surface roughness of zinc indium oxide (ZIO) thin films and observed the
minimum roughness for 0.5 RF/DC ratio and maximum for 1 RF/DC ratio [33].
It is clear from the above discussion that surface roughness, residual stress and electrical
conductivity need a different set of growth parameters to optimize their properties for flexible
OLED applications. The one-parameter-at-a-time approach is not appropriate to search a
common growth space to optimize surface roughness, residual stress and electrical
conductivity in a-IZO thin films. Therefore, we have to condsider the interaction of growth
parameters that may help us to find a common growth space to optimize these properties
simultaneously. We have adopted a method to investigate the effect of growth parameters and
their possible two-way and three-way interactions. To achieve this, we used Minitab 17
statistical software to revisit the growth space. All the data of surface roughness, residual
stress and electrical conductivity from Table 1 is fed into Minitab 17 software for further
analysis. Regression models and analysis of variance (ANOVA) were used to investigate the
influence of primary growth parametrs and their interactions on the output result [34]. The
regression model established a relationship among the different variables, accounting for the
variation of the output between the end points of the two level system. A P-value with a fixed
significance level of 0.05, signifying a 95% confidence level in the result, was used as the
minimum significance level to include any growth parameters and their interactions in the
regression model and ANOVA analysis. Figure 4 shows half-normal plots generated from the
regression model and ANOVA analysis; it depicts the correlation and anti-correlation of
growth parameters on the surface roughness. The red data points (filled square) are
significant while black data points (filled sphere) close to the solid blue line do not
significantly impact the surface roughness. For surface roughness (Figure 4), the two-way
interaction between growth pressure (Pr) and RF/DC ratio (RF/(RF+DC)) is the dominating
growth parameter. It has the highest impact on the surface roughness of a-IZO thin films.
Power (P)-growth pressure (Pr) is the second and growth pressure (Pr)-oxygen partial pressure
(PO2)-RF ratio (RF/(RF+DC)) is the third most dominating two way and three way
interactions of growth parameters to impact surface roughness. From the previous study, it
was established that for residual stress in a-IZO thin films growth pressure was the most
significant growth parameter followed by the three-way interaction among power-oxygen
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partial pressure-RF/(RF+DC)[25]. On the other hand, for electrical conductivity,
RF/(RF+DC) was the most significant growth parameter, followed by sputtering power and
growth pressure. It is clear from here that there are no growth parameters that can be
maximized or minimized to simultaneously optimize surface roughness, residual stress and
electrical conductivity for IZO thin films.
FIG. 4. Half normal plot of the absolute standardized effect for surface roughness. Red data
points (filled square) are significant while black ones (filled sphere) are not significant. A, B,
C and D correspond to power, growth pressure, oxygen partial pressure and RF/DC ratio,
respectively.
To predict the behaviour of surface roughness for a-IZO thin films, an empirical relation
depending on controlled growth parameters, and their two- and three-way interaction were
developed. If the system response follows the assumption of linearity between lower and
upper limits of the growth parameters, this empirical relation can be used to predict the
surface roughness for a-IZO thin film grown within the experimental growth conditions. The
model equation for surface roughness is as follows:
0.34  0.001P  0.02 PP  0.25PO2  1.61RF /( DC  RF )  0.0011P  PP  0.0028P  PO2

 0.001P  RF /( DC  RF )  0.029 PP  PO2  0.22 PP  RF /( DC  RF )  2.33PO2  RF /( DC  DC)
 0.0006 P  PP  PO2  0.0004 P  PP  RF /( DC  DC)  0.005P  PO2  RF /( DC  RF )
 0.268PP  PO2  RF / DC
To verify the empirical regression model equation, we generated contour plots from the
above mentioned equation, as shown in Figure 5. Since, two-way interaction among
sputtering power, growth pressure and RF/(RF+DC) are the most significant parameters to
impact the surface roughness, we varied sputtering power and growth pressure to explore the
11
contour plot and kept oxygen partial pressure and RF/(RF+DC) ratio at low and high,
respectively. In this plot there are four corner points, sputtering power of 25 W and 150 W at
deposition pressures of 4 mtorr and 10 mtorr with the fixed value of oxygen partial pressure
and RF/(RF+DC) ratio at 1% and 1, respectively. The four corner points with predicted
values from the regression model equation are compared with the experimentally achieved
values (in parenthesis).
0.75 nm 1.54 nm
(0.83±0.07) (1.92±0.13)
1.75 nm
0 nm
0.98 nm 0.36 nm
(0.95±0.09) (0.26±0.02)
FIG. 5. Contour plots for the variation of surface roughness with sputtering power and growth
pressure generated by empirical model equations. The oxygen partial pressure and RF/DC
ratio are held constant at 1% and 1, respectively.
The green region was labelled for the surface roughness value of ≤0.5 nm. As the power is
increased at constant growth pressure and at a fixed value of oxygen partial pressure and
RF/DC ratio, the surface roughness decreases and a small green region appears in the corner
with the surface roughness of 0.26±0.02 nm. Furthermore, surface roughness was more than
0.5 nm in rest of the growth space. The close matching of the predicted and experimentally
measured values of surface roughness in the four rectangles validates the regression model
equation.
From Figure 5 it is clear that for low surface roughness the growth pressure and oxygen
partial pressure should be low while the sputtering power and RF/(RF+DC) should be high.
Though for low surface roughness our model provides the necessity of high sputtering power
and low growth pressure but these growth condition may lead to high residual stress in a-IZO
thin films[25]. At higher RF/(RF+DC) ratio, the electrical conductivity was poor, low
RF/(RF+DC) resulted in good electrical conductivity with high residual stress in a-IZO thin
12
films. From previous report, low residual stress and moderate electrical conductivity in a-IZO
thin films was achieved at RF/(RF+DC) ratio of 0.50 and sputtering power of 35 and 50 W.
Therefore, from the previous knowledge and current results, we selected RF/(RF+DC) ratio
of 0.75, in middle of the two (1 and 0.5), and plotted the contour plots for different low PO2,
as shown in Figure 6(a-c). In Figure 6(a-c), the green region is marked for the growth space
that is predicted to yield surface roughness of ≤0.5 nm. It is clear from the figure that as the
oxygen partial pressure increases from 0.1% to 0.5%, the green region recedes towards lower
growth pressure. The lower oxygen partial pressure at high RF/(RF+DC) ratio will have a
low density of highly energetic negatively ions which may help to achieve low residual stress
and moderate electrical conductivity along with low surface roughness. Therefore, we
selected the growth space corresponding to PO2 at 0.1%.
PO2
0.10 0.25(%) 0.50
(a) (b) (c)
FIG. 6. Contour plots for surface roughness when sputtering power and growth pressure are
varied with fixed RF/(RF+DC) of 0.75 and at different PO2 of (a) 0.10%, (b) 0.25% and (c)
0.50%.
Figure 7 (a-b) is the contour plots for surface roughness and residual stress at the proposed
growth condition, PO2 of 0.1% and RF/(RF+DC) of 0.75.
13
(a) (b)
FIG. 7. Contour plots for (a) surface roughness and (b) residual stress with fixed
RF/(RF+DC) and PO2 of 0.75 and 0.10%. The marked solid sphere represent the proposed
growth condition for low surface roughness and low residual stress in Figures (a) and (b),
respectively.
We select the growth space at Power P= 35 W, growth pressure Pr= 5 mtorr, oxygen partial
pressure PO2 =0.1% and RF ratio RF/(RF+DC) = 0.75 for a target surface roughness of ≤0.5
nm, (Marked with solid sphere in Figure 7(a)). The predicted contour plot for residual stress
based on the previous results at the above mentioned growth parameters is shown in Figure 7
(b) with proposed growth condition by solid sphere. The proposed growth conditions for
achieving low surface roughness, low residual stress and moderate electrical conductivity is
shown in Table 2.
The proposed growth condition was tested and IZO thin films were deposited on Corning
glass and flex glass substrates. The surface roughness, residual stress and electrical properties
were measured and the results are shown in Table 2. The roughness of the new sample was
measured and found to be 0.55±0.03 nm. Electrical conductivity and residuals stress were
also measured on samples grown under this condition. The electrical conductivity and
electron mobility were found to be moderate at 1962.22±3.84 S/cm and 35.66±0.12 cm2/Vs,
respectively. The residual stress was measured and found to be -0.52±0.04 GPa.
14
FIG. 8. Atomic force microscopy image (1×1 µm2) for optimized growth condition
(Sputtering power P= 35 W, growth pressure Pr= 5 mtorr, oxygen partial pressure PO2 =0.1%
and RF ratio RF/(RF+DC) = 0.75). Roughness is 0.55±0.03 nm.
Table 2: Proposed growth space to optimize low surface roughness, low residual stress and
moderate electrical conductivity. The measured properties of a-IZO thin films are also listed.
Growth parameters Surface Residual Electrical

roughness stress conductivity
P(W) Pr(mtorr) PO2 (%) RF/(RF+DC) (nm) (GPa) (S/cm)
35 5 0.1 0.75 0.55±0.03 -0.52 ± 0.04 1962.22 ± 3.84
The proposed growth space was found to achieve low residual stress, low surface roughness
and moderate electrical conductivity in a-IZO thin films. Optimizing growth conditions and
understating complex growth spaces can help to improve the properties of TCO electrodes for
OLEDs, photovoltaic and flexible electronics applications.
IV. CONCLUSIONS
Growth conditions for a-IZO thin films were simultaneously optimized to achieve low
residual stress, low surface roughness, and moderate electrical conductivity. The assumption
of low surface roughness for a-IZO does not hold in all growth conditions, as illustrated by
the results shown here. The surface roughness of a-IZO was found to vary from 0.19 nm to
3.7 nm for growth conditions generated by a full factorial DOE matrix of two levels and four
growth parameters. A systematic design of experiments and analysis of variance approach
was used to optimize the growth conditions for low surface roughness, low residual stress and
15
moderate electrical conductivity in a-IZO thin films. The two-way interaction between
growth pressure and RF/DC ratio was the most dominant growth parameter for surface
roughness. An empirical model was developed that successfully predicted a growth space for
low surface roughness. The extrapolation of the growth space, using previous knowledge and
current results, successfully led to low residual stress and moderate electrical conductivity
with target surface roughness in a-IZO thin films. The present study is a useful demonstration
of simultaneous optimization of properties that may be applied in other TCO systems for next
generation flexible device applications.
ACKNOWLEDGMENTS
We sincerely acknowledge department of physics, IIT Ropar for SEED grant and Junior
Research Fellowship. Author (MK) also acknowledges prior use of the National Renewable
Energy Laboratory (Golden, Colorado, USA) facilities to fabricate the IZO thin films used in
our previous work.
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Design of Low Surface Roughness-Low Residual Stress-High Optoelectronic Merit a-IZO Thin Films For Flexible OLEDs

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Design of Low Surface Roughness-Low Residual Stress-High Optoelectronic Merit a-IZO Thin Films For Flexible OLEDs

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Design of low surface roughness-low residual stress-high

optoelectronic merit a-IZO thin films for flexible OLEDs

Corresponding author: mkumar@iitrpr.ac.in and cpackard@mines.edu

II. EXPERIMENTAL DETAILS

S. Growth parameters Residual Electrical Surface

III. RESULTS AND DISCUSSION

To understand the impact of growth parameters on surface roughness, electrical conductivity

0.34  0.001P  0.02 PP  0.25PO2  1.61RF /( DC  RF )  0.0011P  PP  0.0028P  PO2

Growth parameters Surface Residual Electrical

35 5 0.1 0.75 0.55±0.03 -0.52 ± 0.04 1962.22 ± 3.84

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