Highly flexible transparent electrodes for organic light-emitting diode-based displays

Jay Lewis, Sonia Grego, Babu Chalamala, Erik Vick, and Dorota Temple

Citation: Applied Physics Letters 85, 3450 (2004); doi: 10.1063/1.1806559

View online: http://dx.doi.org/10.1063/1.1806559
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 APPLIED PHYSICS LETTERS VOLUME 85, NUMBER 16 18 OCTOBER 2004

Highly flexible transparent electrodes for organic light-emitting

diode-based displays
Jay Lewis, Sonia Grego, Babu Chalamala, Erik Vick, and Dorota Temple
MCNC Research & Development Institute, 3021 Cornwallis Road, Research Triangle Park,
North Carolina 27709-3910, USA
(Received 8 March 2004; accepted 17 August 2004)
Multilayer indium-tin-oxide (ITO)–Ag–ITO stacks were evaluated as transparent conductors for
flexible organic light-emitting diode (OLED) displays. The ITO–metal–ITO (IMI) samples
exhibited significantly reduced sheet resistance over ITO and greater than 80% optical transmission.
The IMI films deposited on plastic substrates showed dramatically improved mechanical properties
when subjected to bending both as a function of radius of curvature as well as number of cycles to
a fixed radius. OLEDs were fabricated on both ITO and IMI anodes, and the devices with IMI
anodes showed improved performance at current densities greater than 1 mA/ cm2 due to the
improved conductivity of the anode. © 2004 American Institute of Physics.
[DOI: 10.1063/1.1806559]

Indium tin oxide (ITO) is the most commonly used elec-
trode material in flat panel displays as it provides good elec-
trical conductivity and high transparency in the visible re-
gion. Moreover, for flat panel displays based on organic
light-emitting diodes (OLEDs), ITO is the preferred anode
material as it provides good energy-level alignment for the
efficient injection of holes into the organic layers.1–3 How-
ever, with the increasing interest in the development of dis-
plays on flexible substrates, there is a great need for a more
mechanically robust flexible transparent conductor as ITO
interconnects fail under lower mechanical strain than the
other device layers.4,5
An alternative to a simple ITO film for transparent con-
ductors is the use of dielectric–metal–dielectric (DMD) mul-
tilayers, also known as ITO–metal–ITO (IMI) when ITO is
used instead of dielectric cladding layers. These structures
are typically composed of a thin silver layer 共⬃10– 15 nm兲
sandwiched between two high dielectric constant layers
共⬃30– 50 nm兲. When designed properly, the high index of
refraction contrast between Ag and the dielectric layers re-
sults in efficient plasmon coupling and visible transparency
greater than 90% can be achieved.6,7 While these structures
have been investigated in detail for applications in heat mir-
rors, low-e window coatings, windshields, electromagnetic
interference shielding,8–13 and have been suggested for im-
proved conductivity electrodes for displays,7,14–17 their utility
as mechanically robust transparent conductive electrodes for
flexible displays has not been reported.
With ITO as the dielectric layer, IMI electrodes are fully
compatible with existing OLED structures, and offer several
advantages over ITO. In addition to improved electrical con-
ductivity, high temperature annealing is not required to
achieve good electrical conductivity so the process is com-
patible with deposition on low temperature polymer sub-
strates.
In this letter we demonstrate the improved performance
of IMI over ITO with regard to conductivity and transpar-
ency. We also show that the addition of the ductile silver
layer provides improved robustness under mechanical strain.
In addition, we report the integration of IMI electrodes with
OLEDs and demonstrate significant improvements in the op-
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82.25.243.173 On: Thu, 22 May 2014 13:47:48
erational characteristics of these devices, especially for high
current densities.
IMI structures were fabricated on 100-␮m-thick
Melinex® polyethylene terephthalate (PET) and Corning
1737 glass substrates. Top and bottom ITO films were rf
magnetron sputter deposited under identical conditions from
a 3-in. target 共90% SnO2 / 10% In2O3兲 at a rate of
0.2 nm/ sec. Sputter conditions were optimized to provide
sufficient conductivity for OLED devices on PET
共⬍100 ⍀ / sq兲 at room-temperature deposition, with a sec-
ondary consideration for transparency. Sputter deposition
was performed with a rf power of 50 W, pressure of
8 mTorr, and gas flow rates of 0.1 SCCM O2 and
99.9 SCCM Ar, where sccm denotes cubic centimeter per
minute at STP. Ag films were deposited by electron beam
evaporation at room temperature, again at a deposition rate
of 0.2 nm/ s. ITO film thickness was calibrated using spec-
troscopic ellipsometry and Ag film thickness was monitored
during deposition with a quartz crystal microbalance and
calibrated using a stylus profilometer. All films were depos-
ited sequentially without breaking vacuum. Unless otherwise
noted, IMI samples were fabricated using 35-nm ITO for
each layer with the Ag layer sandwiched in between. The
effect of Ag layer thickness on optical, electrical, and me-
chanical performance was studied using thicknesses of 0, 4,
8, 12, and 15 nm.
The transmission spectra for the IMI samples were very
similar in character to those in Ref. 15, with transmission
rather flat in the visible and gradually decreasing at both the
red and blue ends of the visible spectrum. Average transmis-
sion in the 450– 650-nm range, Tavg, as a function of Ag film
thickness is shown in Fig. 1. ITO films on PET without a Ag
layer showed Tavg of 74.6%, whereas IMI structures with Ag
layers showed Tavg values between 66.0% and 76.9%. The
highest Tavg values were obtained for Ag films with thickness
in the 8 – 12-nm range.
With the addition of a Ag layer to the structure, signifi-
cant improvement in conductivity was anticipated. Sheet re-
sistance Rs was measured using the four-point probe tech-
nique, and the data are shown in Fig. 1. Compared to ITO
films, IMI samples showed improved electrical conductivity,
3450 © 2004 American Institute of Physics
 Appl. Phys. Lett., Vol. 85, No. 16, 18 October 2004
FIG. 1. The top plot shows the results of measuring two-point resistance as
a function of the bend radius. R10 and the corresponding strain are given as
a function of Ag layer thickness. The bottom plot shows Tavg, and Rs as a
function of Ag film thickness for IMI multilayers on glass and PET
substrates.
with Rs decreasing with increasing Ag thickness. For ex-
ample, with a 12-nm Ag film in the IMI, electrical conduc-
tivity improved by over 15 times. Improvement in the elec-
trical conductivity was obtained with Ag films as thin as
4 nm, where a continuous Ag layer is not observed. The Rs 17
values were consistently lower by ⬃10% for films deposited
on glass compared to those on PET. The data demonstrate the
advantage of IMI multilayers in achieving low Rs values
with low temperature processing.
Measurements of the effect of bending were made by
clamping the sample in a semicircle between two parallel
plates. One plate was fixed to a rigid support, while the other
plate was mounted to the drive shaft of a stepper motor.
Samples with 50-mm length and 5-mm width were clamped
between the two plates with the conductor on the outside at
an initial radius of 14 mm. In this configuration, the conduc-
tive films are under tensile stress. The bending radius was
approximated as half the distance between the plates. Elec-
trical contact was made by the clamps and resistance was
monitored with a multimeter. To determine the effect of re-
peated bending, the distance between the parallel plates was
changed at a rate of 10 mm/ s.
Bend experiments were performed for multiple samples
of each type as a function of radius and number of cycles. A
10% increase in resistance was used to define the onset of
failure, R10, and the film strain was calculated using Young’s
moduli values of 5, 83, and 118 GPa for PET, Ag, and ITO,
respectively. The results for R10 are shown in Fig. 1 as a
function of Ag layer thickness. As a function of curvature,
the IMI samples with at least 8 nm Ag showed improved
performance, with R10 occurring at a smaller radius of cur-
vature.
While bending performance as a function of radius im-
proved, the performance of IMI structures after many cycles
of bending showed more dramatic improvement over ITO.
The resistance data for samples bent to a radius of 6 mm as
a function of the number of cycles are shown in Fig. 2. The
data shown for each sample type were the best achieved in
our experiments, and give the resistance R as a ratio with the
starting value R0. All samples with at least 8-nm Ag showed
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dramatic improvement in cycling performance. Specifically,
82.25.243.173 On: Thu, 22 May 2014 13:47:48
Lewis et al. 3451
FIG. 2. Change in resistance after repeated bending to r = 6 mm as function
of the number of cycles for ITO and IMI multilayers with Ag thickness of 4
and 12 nm.
after 10 000 cycles the value of R / R0 for the ITO sample was
7.4, while the values for the samples with Ag thickness of 8,
12, and 15 nm were similar, with an average value of 1.22.
Another advantage of the IMI structure over ITO was the
recovery of electrical conductivity after large increases in
resistance due to bending. Resistance was measured after
relaxing each sample from a 3-mm radius of curvature back
to a 14-mm radius. ITO samples increased in resistance to
10–20 times the original value. On the other hand, all IMI
samples with at least 8-nm Ag showed an increase of only
1.2–2.7 times the original value.
The response of IMI multilayers to bending suggests that
the ductility of the Ag layer provided effective electrical con-
ductivity even after the ITO was beyond its failure strain
共⬃0.8% 兲. This is consistent with the properties of bulk Ag,
which fails at elongation in the range of 4%–50% depending
on the preparation of the sample.18 However, the sample with
4-nm Ag showed that without significant interconnectivity in
the Ag layer, bending performance does not improve over
that of ITO. Further experiments are needed to demonstrate
the ductile failure mechanism.
To demonstrate the effect of improved electrical perfor-
mance of IMI electrodes, OLED devices were fabricated on
glass using both ITO and IMI anodes. In order to compare
IMI performance with high-quality ITO, we used ITO with
Rs of 20 ⍀ / 䊐 and Tavg of 82% purchased from Colorado
Concept Coatings, LLC. The IMI layer thicknesses were
40/ 10/ 40 nm (ITO/Ag/ITO), and the resulting film had an
Rs of 10 ⍀ / 䊐 and Tavg of 80%. All other device layers were
deposited simultaneously for both samples. Both anodes
were O 2 -plasma treated prior to organic deposition. The or-
ganic materials were used as received from Kodak. The de-
vice layers were 15-nm CuPc (copper phthalocyanine) as the
hole injection layer, 40-nm NPB
[N , N⬘-bis(naphthalen-1-yl)-N , N⬘-bis(phenyl)benzidine] as
the hole transport layer, and 60-nm Alq3 [tris-(8-
hydroxyquinoline) aluminum] as the electron transport/
emission layer, and 0.8-nm LiF and 100-nm Al as the cath-
ode. Devices were encapsulated in a N2 ambient before
characterization. Current–voltage measurements were per-
formed using a Keithley 2400 SourceMeter and luminance–
voltage measurements were performed using a calibrated Si
photodiode.
The luminance and current are shown as a function of
voltage in Fig. 3. The current data show that at low voltages
the two devices behaved nearly identically, which was ex-
 3452 Appl. Phys. Lett., Vol. 85, No. 16, 18 October 2004
FIG. 3. Luminance and current as a function of voltage for OLEDs using
ITO and IMI multilayers as the anode.
pected since the chemical nature of the injection layer for the
two samples was similar. A difference between the samples
appeared for current densities above 1 mA/ cm2 where ohmic
losses in the ITO anode became significant. For our devices,
the ITO sample reached a current density of 300 mA/ cm2 at
10.3 V, while the same current density was achieved in the
IMI sample at 8.9 V. This difference in applied voltage is
explained by accounting for ohmic losses of 70 ⍀ and 33 ⍀
in the anode lines, respectively. The resulting voltages across
the devices were identical at 7.8 V. For other devices the
magnitude of improvement in performance by using IMI de-
pends on the particular geometry and resistance of the anode
transmission line in the OLED. There appeared to be no
influence of anode type on the maximum cd/A efficiency
(typically 4.5 cd/ A), but lum/W efficiency improved by re-
ducing ohmic losses; at a luminance of 10 000 cd/ m2 the
lum/W efficiency of the IMI sample improved by 22% com-
pared to that of the ITO sample. The reduction in ohmic
losses in the anode is especially advantageous for high-
brightness and passive-matrix displays where higher momen-
tary brightness is necessary, and ITO transmission lines are
long and narrow.
The electroluminescence (EL) spectra for OLEDs on
ITO and IMI anodes were measured as a function of the
angle using a Photoresearch SpectraScan 705 spectroradiom-
eter. Minor changes in the EL spectra are seen with different
anodes due to a change in optical cavity structure, and the
data showed that the angular dependence of emission spec-
trum for both ITO and IMI anodes was minimal. For the ITO
sample measured between 0° and 70° angle of incidence, the
maximum emission wavelength shifted from
522 to 526 nm, and the full width at half maximum
(FWHM) of the emission peak increased by 3 nm. For the
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82.25.243.173 On: Thu, 22 May 2014 13:47:48
Lewis et al.
IMI sample the peak shifted from 527 to 526 nm and the
FWHM decreased by 2 nm in the same range of angle of
incidence.
IMI structures showed promise for use as a transparent
conductor in flexible displays. They provided significantly
reduced sheet resistance compared to ITO, and improved
bending properties both as a function of radius and as a func-
tion of cycling. Excellent performance in transmission, con-
ductivity, and bending was obtained from an 8- to 12-nm Ag
layer between 35-nm ITO layers. Even after severe bending
to a 3-mm radius the electrical resistance of IMI structures
increased by only 1.2–2.7 times after relaxing, making them
far more robust for handling and processing. OLED devices
fabricated on an IMI anode showed improved performance
for current densities greater than 1 mA/ cm2 over similar de-
vices using an ITO anode due to the increased conductivity
of the anode.
The authors gratefully acknowledge support for this
work from the Army Research Laboratories.
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