Organic Electronics 32 (2016) 27e33

Contents lists available at ScienceDirect

Organic Electronics
journal homepage: www.elsevier.com/locate/orgel

Polymer-based scattering layers for internal light extraction from

organic light emitting diodes
Daniel Riedel a, b, *, Thomas Wehlus a, Thilo C.G. Reusch a, Christoph J. Brabec b, c
a
OSRAM OLED GmbH, Wernerwerkstrasse. 2, D-93049, Regensburg, Germany
b €t Erlangen-Nürnberg - Materials for Electronics and Energy Technology (i-MEET), Martensstrasse 7, D-91058, Erlangen,
Friedrich-Alexander-Universita
Germany
c
ZAE Bayern e.V., Bereich Erneuerbare Energie, Haberstrasse 2a, D-91058, Erlangen, Germany

a r t i c l e i n f o a b s t r a c t

Article history: Efficient light extraction for organic light emitting diodes (OLED) using scalable processes and low-cost
Received 7 December 2015 materials are important prerequisites for the future commercialization of OLED lighting devices. The
Received in revised form light-extraction technology exhibited in this paper uses polymer-based high-refractive index scattering
5 February 2016
layers processed from solution. The scatter matrix formulation incorporates two types of nanoparticles
Accepted 6 February 2016
Available online xxx
for refractive index tuning and scattering, respectively. Planarization by the same material in order to
reduce surface defects was critical for achieving highly increased device yield. Highly efficient and
defect-free large-area (1.8 cm2) white OLED devices were fabricated on top of the scattering layer in a
Keywords:
Organic light-emitting diodes
bottom emitter configuration. Light extraction enhancement leads to an overall efficiency gain of up to
Internal light extraction 81% for luminances of 5000 cd m
2.
Scattering layers © 2016 Elsevier B.V. All rights reserved.
Planarization
OLED

1. Introduction transparent anode (indium tin oxide - ITO). Around 30% is trapped
in the glass substrate and ~50% in the high refractive index region of
Today, organic light-emitting diodes (OLEDs) are a promising the ITO/organic layers [4]. Hence, only ~20% of the generated light
technology for the future of illumination. OLED's unique features can escape the device. The angular range in that the escaping light
like transparency, flexibility and thinness offer new possibilities for propagates is called the escape cone. By adding a light extraction
design and application. However, to be competitive with conven- layer, the trapped light can be redistributed, so that some of it also
tional light sources, the price per lumen needs to be reduced [1]. reaches the escape cone.
Increasing light extraction is an appropriate approach to increase The light trapped in the substrate can be accessed using external
the performance of the device [2]. However, the additional cost of extraction on the side of the substrate that faces air. Common
light extraction measures should be kept to a minimum. Many techniques are micro lens arrays or scattering layers attached to the
schemes for increasing the light extraction in OLEDs have been substrate after processing the OLED devices on the opposite site of
proposed [3]. In this work, we present an outcoupling technology the substrate [5,6] The substrate modes and the ITO/organic-modes
for internal light extraction which combines the benefits of low- can be redistributed by introducing internal light extraction layers
cost materials, scalable processes, and high efficiency gain. (IEL), which results in enhanced light out-coupling [3,7,8]. To access
Due to the different refractive indices of the substrate (n ~ 1.5) the light trapped inside the organic layers, the refractive index of
and the organic layers (n ~ 1.8) e where light emission takes place e the IEL layers needs to be equal to or higher than that of the ITO/
light is trapped by total internal reflection. The organic layers are organic layers. Equally important for the efficiency gain induced by
sandwiched between a reflective metallic cathode and a the internal light extraction layer are the layer's other optical
properties such as haze and absorption. The lower the absorption of
the IEL, the higher the overall efficiency.
Light scattering, micro lenses or photonic structures can be used
* Corresponding author.
E-mail addresses: [email protected] (D. Riedel), thomas.wehlus@ for internal light recycling [3]. Some of those techniques are either
osram-oled.com (T. Wehlus), [email protected] (T.C.G. Reusch), very expensive or cannot be applied to large areas or high volume
[email protected] (C.J. Brabec).

http://dx.doi.org/10.1016/j.orgel.2016.02.004
1566-1199/© 2016 Elsevier B.V. All rights reserved.
28 D. Riedel et al. / Organic Electronics 32 (2016) 27e33

throughput. A promising low-cost approach with commercial po- wavelength of 550 nm. The refractive index of the matrix of the
tential is the use of volume scattering layers. Shiang et al. already volume scattering layer, shown in Fig. 2 b), is higher or at least equal
presented a deep discussion about the outcoupling of light for to that of the organic layers (n ~ 1.7e1.9) and thus light extraction of
volumetric scattering layers of different haze values [9]. C.-H. Shin both ITO/organic-modes and substrate modes is expected. The
et al. reported scattering layers made of polystyrene with tailored refractive index of the material can be described by the
embedded Al2O3 particles to enhance the light extraction of OLEDs effective medium approach and can be calculated according to the
by 40% [10]. The absolute values of the external quantum efficiency volume fractions of the polymer and the nano-fillers [15]. The
(EQE) were conducted at a current density of 53 mA cm
2 and are extinction coefficient, also shown in Fig. 2 b), is below <10
3 in the
raised from 1.2% to 1.8%. For further improvement an index- region of the typical OLED emission spectrum, between 450 and
matched scattering medium is needed, to access and redistribute 700 nm, which is sufficiently low in order to neglect absorption
wave-guided ITO/organic modes. Chang et al. reported a fourfold losses. Beside optical properties, such as absorption within the
power efficiency improvement at 5000 cd m
2 of blue phospho- scattering layer by either the polymer matrix or scattering particles,
rescent OLED by using nanocomposite scattering layers with high the surface quality of the IEL is a key requirement for zero-defect
refractive index, which consist of a transparent photoresist and OLED deposition. This is the most critical attribute when applying
TiO2 particles in two different sizes [11]. Small particles with a size the particle-based polymeric scattering layer to OLEDs. Due to the
of 25 nm were used to raise the refractive index and larger particles architecture, all of the active layers were deposited on top of the
to induce scattering. Blue-emitting OLED devices were manufac- scattering layer. Each topological defect can lead to an electrical
tured on top of the scattering layers with an active area of defect in the OLED devices. Both spikes and holes in the surface of
2  2 mm2. The external quantum efficiency (power efficacy) of the IEL represent critical defects for further OLED processing. To
those devices at 1000 cd m
2 were raised to 25.2% (37.1 lm W
1) reduce roughness, spikes and holes, a planarization layer is intro-
compared to 11.0% (11.6 lm W
1) of the reference with a strong roll- duced on top of the IEL. It is made of the same high refractive index
off for higher luminances. The resulting gain factors showed a material used for the matrix of the scattering layer, but without the
strong variation with current density. The results are promising but dispersed scatter particles. Therefore it is perfectly index-matched
do not show if the technology is applicable on large areas with a to the IEL and has no effect on light extraction capabilities,
high production yield. In the present work, a similar nano- neglecting general absorption.
composite material system is evaluated and the results are shown To evaluate the surface quality of the IEL and the planarized IEL
on larger areas, with a statistic of plenty manufactured white-light respectively, Atomic Force Microscope (AFM) and Scanning Elec-
emitting OLED devices to show the need for planarization layers on tron Microscope (SEM) measurements were obtained. The AFM and
those composite scattering layers, in order to achieve high pro- SEM images of the IEL and the planarized IEL are shown in Fig. 3.
duction yield. The overall roughness is dramatically reduced by the planarization
Besides refractive index matching of the IEL, the surface layer. For a 20  20 mm2 area measured by AFM, the root-mean-
roughness and especially surface defects are critical properties square roughness was reduced from 35 nm to 7 nm. In other
[12e14]. Both holes and spikes can result in electrical defects or words, planarization reduces roughness by a factor of 5. It should be
short circuit the OLED devices deposited on the IEL. Each electrical noted that the roughness was only measured on a small area and is
defect leads to a device failure. For general illumination, large therefore merely an indicator that the layer may be usable for
emitting areas are needed, and thus the surface of the IEL layer further OLED deposition. For a complete validation of the surface
must be defect-free on a large scale. Most of the current publica- quality, the OLED device itself is the best test vehicle, as surface
tions evaluate IEL layers on very small OLED areas, and so if irregularities will result in shunts and easily detectable optical
considered for the large areas required for commercialization, artifacts.
many of the presented techniques are too complex, hard to
manufacture, very expensive, or not feasible for high volume 2.2. Analysis of OLED devices
throughput. This work consequently concentrates on low-cost
materials and processing and exhibits the potential for future White-emitting OLED devices, with an active area of 1.8 cm2,
application to large area OLED devices. were fabricated on the pure (device type I) and planarized (device
type II) IEL. Devices with the same stack and size, without any
2. Results and discussion additional layer between the glass substrate and the active stack,
were fabricated as a reference. An overview of the used device
2.1. Analysis of the scattering layers structures is shown in Fig. 1. A tandem structure was used [16], with
a phosphorescent yellow emission unit (Y unit) and a fluorescent
A scattering layer needs to fulfill several requirements in order blue (B unit) one separated by a charge generation layer (CGL)
to be used as an internal light extraction layer in OLED devices. The [17,18]. Electron and hole injection layers (EIL/HIL) and electron and
requirements for the particular device architecture, shown in Fig. 1, hole transport layers (ETL/HTL) inject charge carriers into the de-
are processing-, surface-quality- and optics-related. Solution pro- vice and transport them to the emission units [19]. The total
cessing is a fast and scalable approach for layer deposition. Many thickness of the organic stack was 509 nm. The layer architecture
different techniques are possible, including offset or inkjet printing, was optimized by simulation to achieve white emission according
slot die coating or doctor blading. to the simulation method presented by D. Setz et al. [20] The
An optical analysis of the two scattering layers used as IEL in optimization was performed for maximum light output to air at a
device type I and II is shown in Fig. 2 a). This angular resolved targeted white color point. It should be noted that our results are
scattering measurement shows similar light distributions for both not specific to the details of the material set used and similar results
layer architectures, which indicates that the additional planariza- can be achieved using other OLED stack architectures. For statistics,
tion coating, stacked on top of the scattering layer, does not affect 21 devices each of types I and II were manufactured and seven of
the scattering capabilities. Direct transmission and specular the reference.
reflection for the planarized layer is slightly higher, due to reduced All devices were electro-optically characterized. The cur-
surface roughness and therefore suppressed surface scattering. The rentevoltage characteristics of the three device types are shown in
resulting haze induced by the IEL is ~0.75 (±0.05) evaluated at a Fig. 4 a). All devices exhibit a characteristic diode behavior with
 D. Riedel et al. / Organic Electronics 32 (2016) 27e33 29

Fig. 1. Schematic cross section of the device architecture. The left architecture represents the reference “mirror” device without any IEL. Device type I comprises the same active
layers (ITO, organics, cathode) as the reference, but with an additional IEL layer between the substrate and the ITO anode. Device type II is manufactured with an additional
planarization layer on top of the IEL layer.

1 2.2 1x10
Transmission Reflection refractive index n

E xtinction coefficient (k)

0.1
R efractive index (n)
extinction coefficient k 9x10
2.1
Device type I
Rel. Intensity

0.01 Device type II 8x10

2.0
1E-3 7x10

1.9
1E-4 6x10

1E-5 1.8 5x10

0 20 40 60 80 100 120 140 160 180
a) b)
350 400 450 500 550 600 650 700
Angle /° Wavelength /nm

Fig. 2. a) Angular resolved light distribution of the scattering layers according to the two device types, at a wavelength of 550 nm. b) Refractive index and extinction coefficient of
the polymer-based nanocomposite resin used as matrix for the scattering layer.

Fig. 3. Atomic Force Microscope and Scanning Electron Microscope images of the IEL (upper region) and the planarized IEL (lower region). The AFM image is merged out of the
distinct AFM measurements of the IEL (device type I) and planarized IEL (device type II), using the same height scale.

turn-on-voltages of 4.8 V. Surface defects and irregularities mani- low defect level. The leakage current density of device type I at 2 V
fest themselves in shunts in large-area OLED devices and thus in is around 0.15 mA cm
2 and is therefore significantly higher than
leakage currents or shorted devices. The leakage current density at that of the reference.
2 V of the reference is below 10
3 mA cm
2, which indicates a very By applying a planarization layer on top of the IEL layer in device
30 D. Riedel et al. / Organic Electronics 32 (2016) 27e33

100
10

Current density / mA cm-²

1
0.1
0.01
1E-3 Reference
1E-4 Device type I
Device type II
1E-5
all device
1E-6
0 1 2 3 4 5 6 7 8
Voltage / V
a) b)

100
10
Current density / mA cm-²

1
0.1
0.01
1E-3
1E-4 Reference
Device type II
1E-5
leaking devices discarded
1E-6
0 1 2 3 4 5 6 7 8
Voltage / V
c) d)
Fig. 4. a) Current density as function of voltage for all devices of types I & II and the reference. b) Schematic top-view of the substrate with all devices and a rating of the leakage
current indicating electrical defects by color code and categories A, B and C (green (A): <2 x average reference level; yellow (B): >¼2 x average reference level; red (C): >¼10 x
average reference level). c) Current density as function of voltage for the remaining devices of type II and reference without discarded devices due to electrical defects. d) Schematic
top-view of the substrate with an overview of discarded and remaining devices with proper electric functionality. (For interpretation of the references to colour in this figure legend,
the reader is referred to the web version of this article.)

type II, the level of leakage current is highly reduced close to the All device failures assigned to group B are statistically distributed
reference level. For driving voltages higher than the turn-on on the substrate as shown in Fig. 4 d). The high roughness of the
voltage, device type I has a lower current density than both other pure IEL layer of type I devices results in high defect level densities
device types. Different sheet resistances of the ITO, sputtered on of all OLED devices. Hence, all OLED devices of type I are fall into
glass for the reference devices (39 U sq
1) and on IEL layer for group C (red). The data of all devices of group B and C (yellow, red),
device type I (58 U sq
1) respectively, might explain this decrease. i.e. all devices with a leakage current at least twice as high as the
The lower current density observed for device type I may occur due average reference level, was discarded for a reevaluation of the
to the lower lateral conductivity of the ITO anode and the subse- currentevoltage characteristics as shown in Fig. 4 c). The discarded
quent voltage drop within the anode. The ITO sputtered on the devices are schematically shown Fig. 4 d). As a result, the cur-
planarized IEL layers used in device type II exhibit a sheet resis- rentevoltage characteristics of the reference and type II devices
tance (44 U sq
1) slightly higher but comparable to the reference, in with planarized IEL show good very agreement even below the
line with the observed high current density for device type II. The turn-on voltage, which indicates that the planarization completely
difference in sheet resistance between device type I and II may be smoothes the underlying IEL layer. This critical processing step
due to the influence of the growth surface morphology on the ITO enables a production yield improvement from 0% for device type I
layer. Nucleation effects induced by subsurface TiO2 particles in to 75% for device type II and is therefore seen as a critical step for
type I could explain higher sheet resistances and higher injection the commercialization of volumetric particle-based scattering
barriers as compared to type II. layers for large area OLED devices.
Considering the current density at a bias of 2 V for each device
and sorting them in three groups (green (A): <2 x average reference 2.3. Electro-optical results and efficiencies
level; yellow (B): >¼ 2 x average reference level; red (C): >¼10 x
average reference level) results in the color-coded device map Electro-optical measurements of the fabricated devices are
shown in Fig. 4 b). Devices according to group A (green) can be discussed in this section. All optical measurements were conducted
considered free of electrical defects. Small defects occur due to with an integrating sphere. With turn-on voltages of 4.8 V ac-
small particles or surface defects on the substrate layers. These are cording to the currentevoltage characteristics in Fig. 4 c), the
responsible for elevated leakage currents and are represented by luminance curves in Fig. 5 a) follow typical behaviors. Taking into
group B (yellow). Rough surfaces of the substrate layers or larger account the same current density at the same voltage for both
particles result in electrical defects leading to very high leakage reference and type II devices, the outcoupling of trapped ITO/
currents or short circuits. These devices are represented by group C organic as well as substrate modes results in higher luminance
(red). One of the reference devices seems to have a small defect as values of device type II compared to the reference. The emission
well as 6 of the 21 devices of type II and belong therefore to group B. spectra at different angles of incidence for the reference and device
 D. Riedel et al. / Organic Electronics 32 (2016) 27e33 31

60

Device type II Device type II

10000 Reference
Reference

Luminous efficacy / lm W-1

50

Luminance / cd m-2
1000

40
100

30
10

1 20
3 4 5 6 7 8 0 1000 2000 3000 4000 5000

Voltage / V Luminance / cd m-²

a) b)
0.07 0.07
Reference Device type II
0.06 0° 0.06 0°
Radiance / W sr-1m-2nm-1

Radiance / W sr-1m-2nm-1
15° 15°
0.05 30° 0.05 30°
45° 45°
0.04 60° 0.04 60°
0.03 0.03

0.02 0.02

0.01 0.01

0.00 0.00
400 500 600 700 400 500 600 700
c) Wavelength /nm d) Wavelength /nm

Fig. 5. a) Luminance as function of voltage for the reference and planarized IEL type II devices. b) Luminous efficacy at different luminance values for the reference and planarized
IEL type II devices. c) Emission spectra at different angles of incidence of the reference. d) Emission spectra at different angles of incidence of device type II.

type II are given in Fig. 5 c) and d). The reference shows a strong guided modes are filled with energy which might result in a gain
angular dependent spectra with changes over the whole wave- factor roll-off.
length range. By introducing the scattering layer in device type II
the spectra are nearly angular independent and conduct significant
higher radiances. Slight superimposed modulations occur due to 3. Conclusion
thin film interference effects within the planarization layer.
Luminous efficacy at different luminance levels is shown in Fig. We present an effective and scalable technology to increase the
5 b). At 1000 cd m
2, the reference obtains 32 lm W
1 and device internal light extraction in OLED devices. The technology is based
type II 53 lm W
1. An efficiency roll-off, due to losses for higher on polymeric high-refractive index scattering layers deposited from
current densities, leads to a decrease of the luminous efficacy at solution on the substrate for OLEDs in a bottom-emitting configu-
higher luminance [21]. Additional light extraction induced by the ration. An efficiency gain of up to 1.81 at 5000 cd m
2 and a con-
volume scattering layer leads to an efficiency gain of 1.67 at stant gain of 1.6 for the EQE at constant driving current density
1000 cd m
2, 1.71 at 2000 cd m
2 and 1.81 at 5000 cd m
2. The were demonstrated for white-light-emitting OLED devices with an
increasing gains for higher luminances are the result the compar- active are of 1.8 cm2. Compared to published values for light
ison at same brightness levels. The reference and the type II devices extraction of white-emitting OLED devices the enhancement is
with light extraction operate at different points of the cur- further improved by reducing absorption losses inside the IEL and
rentevoltage characteristic to obtain the same external brightness the OLED stack itself. This key parameters according to the theory of
level: OLED devices with light extraction require less current den- light extraction considers the absorption losses inside the organic
sity to generate the same luminous flux as devices without light stack together with the limited reflectivity of the cathode in the
extraction. Hence, the devices with light extraction are less affected combined effective reflectivity [23]. The simulated effective
by the before mentioned efficiency roll-off: In general, the more reflectivity of the used multilayered OLED stack including ITO and
current flows, the more quenching occurs, leading to a decrease of the cathode exhibit a mean value of 80% over an averaged wave-
luminous efficacy [22]. In other words, overall non-radiative losses length range of 400e750 nm and averaged angles from 0 to 90 .
are reduced due to the decreased amount of injected charge car- Improving this entity is one of the most critical parameter to
riers that are required to operate the device at a given brightness. enhance light extraction with scattering layers.
The comparison of the EQE at a constant driving current density is Surface roughness is a key factor in OLED device yield. We
the best values to evaluate light extraction capabilities. The EQE demonstrate a drastically improvement of the device yield from 0%
values of the reference and devices of type II are given in Table 1. to 75%, considering high leakage currents as device failures, by
They exhibit a comparable roll off and result in a nearly constant adding a planarization layer of the same material as the matrix
gain factor of 1.6 for all current densities. This consistency is a hint material of the scattering layer. Because it is inherently perfectly
for a well optimized stack design because no hidden internal wave index-matched, it has no adverse optical effect on light extraction.
Polymeric scattering layers and the respective processes show
32 D. Riedel et al. / Organic Electronics 32 (2016) 27e33

Table 1
External quantum efficiencies conducted at a constant driving current density of the device type II with the planarized IEL compared to the reference and the resulting gain
factors.

Current density [mA cm
2] EQE [%] (reference) EQE [%] (device type II) Gain factor

1 22.3 36.2 1.63

2 22.3 36.2 1.62
5 21.8 35.1 1.61
10 20.8 33.5 1.61
20 19.2 30.9 1.61

potential for cost-efficient production. For commercialization, the Acknowledgments

in-line production yield needs to be further improved and process
development on coating and dispersion of the nanocomposite The authors acknowledge financial support by the German
scattering material needs to be done. The use of those IEL is not Federal Ministry of Education and Research (BMBF) under the
limited to bottom-emitting OLED devices but may also extend to contract FKZ 13N12240 (project “OLYMP”).
top-emitting and flexible OLEDs in the future.

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