nanomaterials

Article
Enhanced Light Extraction from Bottom Emission
OLEDs by High Refractive Index Nanoparticle
Scattering Layer
Chan Young Park and Byoungdeog Choi *
Department of Electrical and Computer Engineering, Sungkyunkwan University, 2066 Seobu-Ro, Jangan-Gu,
Suwon, Gyeonggi-do 16419, Korea
* Correspondence: bdchoi@skku.edu




Received: 31 July 2019; Accepted: 26 August 2019; Published: 31 August 2019


Abstract: High refractive index nanoparticle material was applied as a scattering layer on the
inner side of a glass substrate of a bottom emission organic light emitting diode (OLED) device
to enhance light extraction and to improve angular color shift. TiO2 and YSZ (Yttria Stabilized
Zirconia; Y2 O3 -ZrO2 ) were examined as the high refractive index nanoparticles. The nanoparticle
material was formed as a scattering layer on a glass substrate by a coating method, which is generally
used in the commercial display manufacturing process. Additionally, a planarization layer was
coated on the scattering layer with the same method. The implemented nanoparticle material and
planarization material endured, without deformation, the subsequent thermal annealing process,
which was carried out at temperature ranged to 580 ◦ C. We demonstrated a practical and highly
efficient OLED device using the conventional display manufacturing process by implementing the
YSZ nanoparticle. We obtained a 38% enhanced luminance of the OLED device and a decreased
angular color change compared to a conventional OLED device.

Keywords: OLED; light extraction; outcoupling; nanoparticle; high refractive index; scatter; efficiency;
display; YSZ

1. Introduction
In flat-panel display devices, organic light emitting diodes (OLEDs) are widely used, from mobile
phones to large size TVs because OLED has excellent electro-optical properties for display products
compared to widely used liquid crystal displays (LCDs). Among the properties, the efficiency of OLED
devices is an important factor for practical OLED display products.
There are many studies on enhancing the efficiency of OLEDs in various technology fields, such
as materials, device structures, fabrication processes, circuit design, and circuit driving. The efficiency
of OLEDs has been enhanced by improving the characteristics of organic materials comprised in OLED
devices and by optimizing the structures of OLED devices [1–4]. However, other approaches for
finding solutions for the improvement of the outer structures of OLED devices have been studied in
order to enhance the efficiency of OLED devices [5,6].
As shown in Figure 1, 20% of emitted light is extracted outside of OLED devices; however, 80% of
emitted light is trapped inside OLED devices and dissipated, which is caused by the difference of the
refractive index of each layer comprised in OLED devices [5,7]. Various ways were tried to extract the
trapped light from the OLED devices [5–7]. Several methods have been proposed to enhance the light
extraction from OLEDs, including mesh structures on the glass substrate [8], silica micro spheres [9],
scattering layers [10], embedded low-index grids [11], photonic crystals [12,13], micro pyramids [14],
and micro lens arrays [15–18]. However, these methods could be used for limited applications such

Nanomaterials 2019, 9, 1241; doi:10.3390/nano9091241 www.mdpi.com/journal/nanomaterials

Nanomaterials 2019, 9, 1241 2 of 9

Nanomaterials 2019, 9, 1241 2 of 9

as illumination products without pixels. Most methods for enhancing the efficiency of OLED are
are implemented on the outer side of the glass substrate, where the distance between the light source
implemented on the outer side of the glass substrate, where the distance between the light source and
and the emitting structures is relatively long, due to the thickness of the glass substrate. In display
the emitting structures is relatively long, due to the thickness of the glass substrate. In display products
products with many pixels, these methods cause image blurring, which is a mixture of light from
with many pixels, these methods cause image blurring, which is a mixture of light from adjacent pixels
adjacent pixels and poor image quality by a diffusion effect. Other approaches have been studied to
and poor image quality by a diffusion effect. Other approaches have been studied to enhance the light
enhance the light extraction of OLEDs, adopting nano sized structures to OLEDs. By the scattering
extraction of OLEDs, adopting nano sized structures to OLEDs. By the scattering effect of the nano
effect of the nano structures, such as gratings [19,20], metallic nanoparticles [21–25], and buckled
structures, such as gratings [19,20], metallic nanoparticles [21–25], and buckled substrates [24,26,27],
substrates [24,26,27], the light trapped in glass substrate can escape. However, nano structures have
the light trapped in glass substrate can escape. However, nano structures have limited application in
limited application in OLEDs due to the complicated process, requiring high cost. Additionally, their
OLEDs due to the complicated process, requiring high cost. Additionally, their size limitation impedes
size limitation impedes their implementation in practical OLED products. Hence, the nanoparticles
their implementation in practical OLED products. Hence, the nanoparticles fabricated by easy methods
fabricated by easy methods or by methods compatible with conventional manufacturing processes
or by methods compatible with conventional manufacturing processes suitable for large areas are more
suitable for large areas are more beneficial for practical OLEDs devices.
beneficial for practical OLEDs devices.
In this study, we applied high refractive index nanoparticle material as a scattering layer on the
In this study, we applied high refractive index nanoparticle material as a scattering layer on the
inner side of the glass substrate of the bottom emission OLED device to enhance light extraction and
inner side of the glass substrate of the bottom emission OLED device to enhance light extraction and to
to improve angular color shift. The nanoparticle scattering layer is located near the emitting layer of
improve angular color shift. The nanoparticle scattering layer is located near the emitting layer of the
the OLED device, compared to previous approaches mentioned above, so it rarely affects the image
OLED device, compared to previous approaches mentioned above, so it rarely affects the image quality
quality of the OLED display. We demonstrated a practical highly efficient OLED device using the
of the OLED display. We demonstrated a practical highly efficient OLED device using the conventional
conventional display manufacturing process by implementing the YSZ nanoparticle as the high
display manufacturing process by implementing the YSZ nanoparticle as the high refractive index
refractive index scattering layer. We obtained a 38% enhancement of luminance of the OLED device
scattering layer. We obtained a 38% enhancement of luminance of the OLED device and a white
and a white angular dependency (WAD) of 0.005 at 60 degrees from normal direction.
angular dependency (WAD) of 0.005 at 60 degrees from normal direction.

Figure 1. Schematic diagram of multi-layer OLED structure and optical ray diagram of light propagation
Figure 1. Schematic diagram of multi-layer OLED structure and optical ray diagram of light
via various modes, i.e., substrate escape, substrate wave guided mode, and ITO/Organic wave
propagation via various modes, i.e., substrate escape, substrate wave guided mode, and ITO/Organic
guided mode.
wave guided mode.
2. Materials and Methods
2. Materials and Methods
TiO2 and YSZ (Yttria Stabilized Zirconia; Y2 O3 -ZrO2 ) were investigated as high refractive index
TiO2 andmaterials
nanoparticle YSZ (Yttriafor Stabilized Zirconia;
scattering layer. TheYrefractive
2O3-ZrO2) index
were investigated as high refractive
of TiO2 nanoparticles is 2.5 andindex
that
nanoparticle
of YSZ is 2.13,materials for scattering
respectively. Both TiOlayer.
2 and The
YSZ refractive
nanoparticlesindex of
are TiO 2 nanoparticles
suitable for high is 2.5
refractiveand that
index
of YSZ is 2.13, respectively. Both TiO and YSZ nanoparticles are suitable for high
materials compared to that of glass substrate. The size of the TiO2 nanoparticle was 250–300 nm, while
2 refractive index
materials
the size ofcompared to that of glass
the YSZ nanoparticle wassubstrate.
100–150The nm. size of the
The TiO2 nanoparticle
nanoparticles was 250–300
were dispersed nm, while
in propylene
the size of the YSZ nanoparticle was 100–150 nm. The nanoparticles were
glycol methyl ether acetate (PGMA) solvent for applying to the slit coating method, which is used dispersed in propylene
glycol
in methyl ether acetate
the conventional display(PGMA) solvent for
manufacturing applying
process to theareas.
for large slit coating method, which
The nanoparticle is used in
suspension
the conventional
was coated on thedisplay manufacturing
glass substrate, formingprocess for large
the high areas.
refractive The scattering
index nanoparticle suspension
layer, followedwas by
coated on the glass substrate, forming ◦
the high refractive index scattering
a thermal curing process at 300–500 C in a furnace for 30 min. The curing temperature can belayer, followed by a thermal
curing process
controlled at 300–500
according to the°C in aoffurnace
state for 30
the coating min.without
layer, The curing temperature can
any deformation. be 2controlled
A SiO solution,
according
which was to the state
normally of the
used coating glass
at spin-on layer,(SOG),
without wasanyuseddeformation. A SiO2 material,
as a planarization solution, which was was
normally used at spin-on glass (SOG), was used as a planarization material, which
coated on the nanoparticle scattering layer. The refractive index of the SiO2 planarization layer was was coated on the
nanoparticle
1.45, which wasscattering
similarlayer. The
to that ofrefractive
the glassindex of the The
substrate. SiO2planarization
planarization layer was was1.45,
formedwhichon was
the
similar to that of the glass substrate. The planarization layer was formed on
scattering layer with the same method as the scattering layer. It was cured at 500 C in a furnacethe scattering
◦ layer with
the same method as the scattering layer. It was cured at 500 °C in a furnace for 30 min. The
planarization layer had a flat surface covering the roughness of the scattering layer caused by the
distribution of nanoparticles. Therefore, subsequent manufacturing process can be performed easily,
Nanomaterials 2019, 9, 1241 3 of 9

for 30 min. 2019,

Nanomaterials The planarization
9, 1241 layer had a flat surface covering the roughness of the scattering layer 3 of 9
caused by the distribution of nanoparticles. Therefore, subsequent manufacturing process can be
performed
like on the easily, like on the
glass substrate glass substrate
surface. Next, the surface. Next,low
conventional the temperature
conventionalpoly low silicon
temperature
(LTPS)polythin
silicon (LTPS) thin
film transistor (TFT)film transistor (TFT)
manufacturing manufacturing
process was performedprocess onwas
the performed
planarization on layer.
the planarization
In the LTPS
layer. In the LTPS TFTprocess,
TFT manufacturing manufacturing process,
the thermal the thermal
annealing annealing
process process
is required is required
at the highestattemperature,
the highest
temperature, ◦
approaching approaching
580 °C, which 580can C, cause
which deformation
can cause deformation of the nanoparticle
of the nanoparticle scatteringscattering
layer and layer
the
and the planarization
planarization layer.
layer. The The proposed
proposed materials
materials shouldshould
endure endure
the highthe temperature
high temperature duringduring
LTPSLTPSTFT
TFT manufacturing
manufacturing process
process without
without any any deformation.
deformation.
A
A conventional
conventional bottom
bottom emission
emission white
white OLED
OLED display
display device
device was was used
used toto investigate
investigate thethe effect
effect
of
of the
the high
high refractive
refractive index
index nanoparticle
nanoparticle scattering
scattering layer,
layer, as
asrepresented
representedin inFigure
Figure2.2. OnOn the
the glass
glass
substrate,
substrate,the
the nanoparticle
nanoparticlescattering
scatteringlayer,
layer,the
theplanarization
planarizationlayer,
layer,andandthe
theTFT
TFTlayer
layer were
were fabricated
fabricated
sequentially.
sequentially. Next, aa color
colorfilter
filterand
andananover
overcoat
coatlayer
layer were
were formed
formed to to reproduce
reproduce color
color images
images on
on the
the OLED display device. On the indium tin oxide (ITO) anode
OLED display device. On the indium tin oxide (ITO) anode electrode, the white electrode, the white OLED device,
device,
comprised
comprisedofofblue,blue,green, and and
green, red emitting layers stacked
red emitting up, wereup,
layers stacked deposited by a thermal
were deposited byevaporation
a thermal
process. The device
evaporation process.wasThefinalized
device with an aluminum
was finalized with cathode and a top
an aluminum glass and
cathode substrate. The size
a top glass of the
substrate.
glass substrate
The size of thewas 370 ×
glass 470 mm.was
substrate Additionally,
370 × 470anmm. OLED device without
Additionally, a nanoparticle
an OLED device scattering
without a
layer and a planarization
nanoparticle scattering layerlayerand
was a also fabricatedlayer
planarization as a reference device. as a reference device.
was also fabricated

Figure2.2. Schematic
Figure Schematic diagram
diagram ofof the
the bottom
bottom emission
emission white
white OLED
OLED device
device with
with the
thescattering
scatteringlayer
layeron
on
the inner side of glass substrate.
the inner side of glass substrate.

Measurements
Measurementsof ofOLED
OLEDproperties
propertieswere
were performed
performed byby recording
recording current–voltage
current–voltage characteristics
characteristics
as well as electro-luminescence (EL) spectra. The current–voltage was
as well as electro-luminescence (EL) spectra. The current–voltage was acquired acquired using
using a Keithley
a Keithley 236
236 voltage source unit, while the EL intensity and spectral characteristics of the devices were measured
voltage source unit, while the EL intensity and spectral characteristics of the devices were measured
with
with aa calibrated siliconphotodiode
calibrated silicon photodiode(Hamamatsu
(HamamatsuPhotonics,
Photonics, Hamamatsu,
Hamamatsu, Japan,S5227-1010BQ),
Japan, S5227-1010BQ),a
aphotomultiplier
photomultipliertube,
tube,and
andaaspectroradiometer
spectroradiometer(Minolta,
(Minolta,Osaka,
Osaka,Japan,
Japan,CS-1000).
CS-1000).

3. Results and Discussion

3. Results and Discussion
3.1. Properties of the Nanoparticle Scattering Layer
3.1. Properties of the Nanoparticle Scattering Layer
The scattering layer with embedded TiO2 nanoparticles was fabricated using the conventional
The scattering layer with embedded TiO2 nanoparticles was fabricated using the conventional
slit coating method. However, TiO2 nanoparticles are hard to disperse in PGMA solvent, therefore
slit coating method. However, TiO2 nanoparticles are hard to disperse in PGMA solvent, therefore
they were not dispersed uniformly. The coating thickness of the TiO2 nanoparticle scattering layer was
they were not dispersed uniformly. The coating thickness of the TiO2 nanoparticle scattering layer
1.5 µm, then 1 µm thick SiO2 was coated as the planarization layer. Table 1 shows the optical properties
was 1.5 um, then 1 um thick SiO2 was coated as the planarization layer. Table 1 shows the optical
of the TiO2 nanoparticle scattering layer, such as transmittance and haze. We observed 70% of total
properties of the TiO2 nanoparticle scattering layer, such as transmittance and haze. We observed
transmittance at 550 nm wavelength and 55–82% of haze. The surface of the TiO2 nanoparticle layer
70% of total transmittance at 550 nm wavelength and 55–82% of haze. The surface of the TiO2
was rough, even though the planarization layer was applied on it. Considering its surface roughness,
nanoparticle layer was rough, even though the planarization layer was applied on it. Considering its
it would cause poor characteristics in the subsequent LTPS TFT process. Due to poor dispersivity of
surface roughness, it would cause poor characteristics in the subsequent LTPS TFT process. Due to
TiO2 nanoparticles in the PGMA solvent, the curing temperature was limited to 300 ◦ C, which was
poor dispersivity of TiO2 nanoparticles in the PGMA solvent, the curing temperature was limited to
lower than the annealing process temperature of 580 ◦ C in the subsequent LTPS TFT process. Despite
300 °C, which was lower than the annealing process temperature of 580 °C in the subsequent LTPS
TFT process. Despite the high refractive index of TiO2 nanoparticles, the use of conditions such as
particle size, sorts of solvent, and better dispersion of TiO2 nanoparticles is required.
Nanomaterials 2019, 9, 1241 4 of 9

the high refractive index of TiO2 nanoparticles, the use of conditions such as particle size, sorts of
solvent, and better dispersion of TiO2 nanoparticles is required.
Nanomaterials 2019, 9, 1241 4 of 9
Table 1. Transmittance and haze of the TiO2 nanoparticle scattering layer.
Table 1. Transmittance and haze of the TiO2 nanoparticle scattering layer.
Layers Total Transmittance (%) Scattering Transmittance (%) Haze
Layers
Scattering layer (1.5 µm) Total Transmittance
70.18 (%) Scattering Transmittance
57.54 (%) Haze
82%
Scattering layer (1.5um) 70.18 57.54 82%
Scattering layer (1.5 µm)
Scattering layer 68.28 37.55 55%
/Planarization layer (1.5um)
(1 µm) 68.28 37.55 55%
/Planarization layer (1um)

On the
On the other
other hand,
hand, the the scattering
scattering layerlayer withwith embedded
embedded YSZ YSZ nanoparticles
nanoparticles was was successfully
successfully
fabricated using
fabricated using the the conventional
conventional slit slit coating
coating method.
method. ZrO ZrO2, comprising YSZ
2, comprising YSZ hashas aa monoclinic
monoclinic crystal
crystal
structure at room temperature. It changes to a tetragonal crystal structure
structure at room temperature. It changes to a tetragonal crystal structure and a cubic crystal structure and a cubic crystal structure
as temperature
as temperature increases.
increases. YSZ YSZ comprised
comprised of of Yttria
Yttria doped
doped ZrO ZrO22 has
has aa stable
stable crystal
crystal structure
structure eveneven
when temperature increases. YSZ has characteristics of chemical
when temperature increases. YSZ has characteristics of chemical stability, thermal resistance, low stability, thermal resistance, low
thermal conductivity, and high strength. It has similar optical properties
thermal conductivity, and high strength. It has similar optical properties to ZrO22, including a high to ZrO , including a high
refractive index.
refractive index. The TheYSZYSZnanoparticle
nanoparticlescattering
scatteringlayer layerwaswas coated
coatedwithwithvarious
variousthicknesses
thicknesses of 1.5ofµm,
1.5
2.5 µm, 4.0 µm, and 7.0 µm, respectively, and then was cured at 500 ◦ C. Next, 1 µm of SiO was coated
um, 2.5 um, 4.0 um, and 7.0 um, respectively, and then was cured at 500 °C. Next, 1 um of SiO2 was 2
as the planarization
coated layer. Figure
as the planarization layer.3Figure
illustrates the morphology
3 illustrates of the YSZ
the morphology ofnanoparticle scattering
the YSZ nanoparticle
layer and the
scattering layer planarization layer including
and the planarization a cross sectional
layer including view, measured
a cross sectional by scanning
view, measured electron
by scanning
microscopy (SEM). The surface of the planarization layer was flat
electron microscopy (SEM). The surface of the planarization layer was flat with small defects, likewith small defects, like the glass
the
substrate.
glass Moreover,
substrate. Moreover,the density of theofYSZ
the density nanoparticle
the YSZ nanoparticlescattering layerlayer
scattering was waslower thanthan
lower thatthat
of the
of
planarization layer. The change of thickness of the planarization layer
the planarization layer. The change of thickness of the planarization layer from 1 um at the coating from 1 µm at the coating step to
0.6 µm after the curing step means that
step to 0.6 um after the curing step means that the coatedthe coated SiO solution permeated into the
2 SiO2 solution permeated into the vacancies vacancies of the
nanoparticle
of scattering
the nanoparticle layer. The
scattering largeThe
layer. difference between refractive
large difference betweenindex of the index
refractive YSZ nanoparticles
of the YSZ
(2.13) and the SiO material (1.45) within the interpenetrating
nanoparticles (2.13) and the SiO2 material (1.45) within the interpenetrating areas enhanced
2 areas enhanced the scattering effect.
the
Table
scattering effect. Table 2 shows optical properties of the YSZ nanoparticle scattering layer.total
2 shows optical properties of the YSZ nanoparticle scattering layer. We obtained 58–78% of We
transmittance
obtained 58–78% of of
thetotal
YSZtransmittance
nanoparticleof scattering layer at 550 scattering
the YSZ nanoparticle nm wavelength layer atand 55024–55% of haze.
nm wavelength
It was observed that transmittance decreased and haze increased as
and 24–55% of haze. It was observed that transmittance decreased and haze increased as the thickness the thickness of scattering layer
was increased.
of scattering This
layer wasmeans that the
increased. Thisthick scattering
means that the layer
thick enhances
scattering thelayer
scatter effect due
enhances the to increasing
scatter effect
light diffusion during its propagation. Therefore, the scatter effect
due to increasing light diffusion during its propagation. Therefore, the scatter effect and and transmittance can be controlled
by modulatingcan
transmittance thebe thickness
controlled of theby scattering
modulating layer.
the Moreover,
thickness of thetheYSZ nanoparticle
scattering layer.scattering
Moreover,layer the
and the planarization layer have ◦ C, so the
YSZ nanoparticle scattering layera anduniform surface and a layer
the planarization high curing
have atemperature
uniform surface of 500and a high
subsequent
curing LTPS TFT
temperature of process
500 °C, so canthebesubsequent
performed easily. LTPS TFT process can be performed easily.

(a) (b)

SEM images
Figure 3. SEM images of
of the YSZ nanoparticle scattering
scattering layer (LSM) and the planarization layer
(LSPM) after the curing process: (a)
(a) Top view of planarization layer; (b) Cross sectional view of the
scattering layer and the planarization layer.
layer.

Table 2. Transmittance and haze of the YSZ nanoparticle scattering layer.

Thickness of Thickness of Total Scattering

Haze
Scattering Layer (um) Planarization Layer (um) Transmittance (%) Transmittance (%)

1.5 1.0 78.43 19.13 24%

2.5 1.0 74.63 20.06 27%

4.0 1.0 65.84 25.47 39%

7.0 1.0 58.43 32.15 55%

Nanomaterials 2019, 9, 1241 5 of 9

Table 2. Transmittance and haze of the YSZ nanoparticle scattering layer.

Thickness of Scattering Thickness of Planarization Total Scattering

Haze
Layer (µm) Layer (µm) Transmittance (%) Transmittance (%)
1.5 1.0 78.43 19.13 24%
2.5 1.0 74.63 20.06 27%
4.0 1.0 65.84 25.47 39%
7.0 1.0 58.43 32.15 55%
Nanomaterials 2019, 9, 1241 5 of 9

3.2. Performance
3.2. Performance of
of the
the OLED
OLED Device
Device with
with High
High Refractive
Refractive Index
Index Nanoparticle
Nanoparticle Scattering
Scattering Layer
Layer
A conventional
A conventionalbottom
bottomemission white
emission OLED
white devicedevice
OLED for flat-panel display products
for flat-panel display was fabricated.
products was
The characteristics of the OLED devices with and without the YSZ scattering layer are
fabricated. The characteristics of the OLED devices with and without the YSZ scattering layer areillustrated as
Figure 4. The
illustrated OLED4.devices
as Figure had three
The OLED peaks
devices had at red,peaks
three green,atand
red,blue color
green, andwavelengths. The OLED
blue color wavelengths.
The OLED devices were used as the light sources to investigate the enhancement of light the
devices were used as the light sources to investigate the enhancement of light efficiency of OLED
efficiency
with an embedded YSZ scattering layer.
of the OLED with an embedded YSZ scattering layer.

(a) (b)

(c) (d)

Figure 4. Characteristics
Characteristics of OLED devices with and without the YSZ scattering layer. The thickness
of the
the YSZ
YSZ scattering
scatteringlayer
layerisis2.52.5um:
µm:(a) (a)
Electroluminescence
Electroluminescence spectrum of the
spectrum of OLED devices.
the OLED The
devices.
spectrum datadata
The spectrum are normalized
are normalizedat 1mA/cm
at 1mA/cm 2 ;Characteristics
2; (b) of luminance
(b) Characteristics for different
of luminance voltages;
for different (c)
voltages;
Characteristics of current
(c) Characteristics density
of current density forfor
different
differentvoltages;
voltages;and
and(d)
(d)Characteristics
Characteristicsofofcurrent
current efficiency
efficiency
for difference luminance.

In the
In the previous
previousstudy,
study,employing
employingaascattering
scatteringlayer
layertotoOLED
OLED devices
devices as as a layer
a layer or film
or film coated
coated on
on outer surface of the glass substrate reported enhanced light efficiency of OLEDs
outer surface of the glass substrate reported enhanced light efficiency of OLEDs [10]. However, the [10]. However,
the distance
distance fromfrom
the the
lightlight emitting
emitting layer
layer to the
to the scattering
scattering layer
layer waswas very
very long,
long, including
including thethe thickness
thickness of
of the glass substrate 0.5 mm compared to the pixel pitch 80 µm. Therefore, the light
the glass substrate 0.5 mm compared to the pixel pitch 80 um. Therefore, the light scatter effect causedscatter effect
caused mixing
mixing colors among
colors among pixels pixels andtoledimage
and led to image
blurblur
on onthethe displayscreen.
display screen.InInthis
this work,
work, wewe
implemented the scattering layer on the inner surface of the glass substrate. The distance from the
light emitting layer to the scattering layer was short, about half of the pixel pitch, so a good image
quality without image blur could be achieved by the proposed method. The emitted light at the OLED
device between the anode electrode and the cathode electrode propagated to various directions while
it passed the scattering layer. The scattered light changed the direction of propagation through the
Nanomaterials 2019, 9, 1241 6 of 9

implemented the scattering layer on the inner surface of the glass substrate. The distance from the
light emitting layer to the scattering layer was short, about half of the pixel pitch, so a good image
quality without image blur could be achieved by the proposed method. The emitted light at the OLED
device between the anode electrode and the cathode electrode propagated to various directions while
it passed the scattering layer. The scattered light changed the direction of propagation through the
glass substrate, which limited the total internal reflection. Therefore, the light from the OLED substrate
Nanomaterials 2019, 9, 1241 6 of 9
wave guided mode could be extracted, which enhanced the light efficiency of the OLED device.
Table 3 shows the relative luminance of OLED devices with the implemented YSZ nanoparticle
Table 3 shows the relative luminance of OLED devices with the implemented YSZ nanoparticle
scattering layer compared to the control device without the scattering layer. In the presence of the
scattering layer compared to the control device without the scattering layer. In the presence of the
scattering layer, the total luminance and luminance in normal direction of the OLED device enhanced,
scattering layer, the total luminance and luminance in normal direction of the OLED device enhanced,
compared to the reference device without the scattering layer. At the thickness of scattering layer,
compared to the reference device without the scattering layer. At the thickness of scattering layer, 2.5
2.5 µm, a 29% enhancement of total luminance and a 38% enhancement of luminance in normal
um, a 29% enhancement of total luminance and a 38% enhancement of luminance in normal direction
direction were achieved. As the result, the optimal thickness of the scattering layer was observed
were achieved. As the result, the optimal thickness of the scattering layer was observed at 2.5 um.
at 2.5 µm. Moreover, the luminance enhancement is not proportional to the increase of the scatter
Moreover, the luminance enhancement is not proportional to the increase of the scatter effect. As the
effect. As the thickness of scattering layer was increased, the luminance decreased. This means that
thickness of scattering layer was increased, the luminance decreased. This means that the
the transmittance of the thick scattering layer lowers as the thickness increases. To analyze optimal
transmittance of the thick scattering layer lowers as the thickness increases. To analyze optimal
thickness of the scattering layer implemented in the OLED device, the luminance change was simulated
thickness of the scattering layer implemented in the OLED device, the luminance change was
using a geometrical optics tracing method. The LightTools program (Synopsys, Mountain View, CA,
simulated using a geometrical optics tracing method. The LightTools program (Synopsys, Mountain
USA)
View,wasCA,used
USA) forwas
the used
simulation.
for theAs Figure 5aAs
simulation. shows, the5a
Figure simplified
shows, the device structure
simplified usedstructure
device for the
simulation also approximated constant values of parameters such as the refractive index
used for the simulation also approximated constant values of parameters such as the refractive index and the
thickness
and the of each layer.
thickness The maximum
of each layer. Theluminance
maximumenhancement was calculatedwas
luminance enhancement as 32% enhancement
calculated as 32%
atenhancement
a thickness of 2.5 µm, in good agreement with the experimental result. Moreover, the
at a thickness of 2.5 um, in good agreement with the experimental result. Moreover, maximum the
luminance
maximumenhancement in normal direction
luminance enhancement was calculated
in normal as 42%
direction was at the center
calculated of the
as 42% device.
at the Figure
center 5
of the
shows
device.the simulation
Figure 5 shows result
the of luminance
simulation change
result in the OLED
of luminance device.
change in the OLED device.
Table 3. Ratio of the luminance of OLED devices with the YSZ scattering layer to the luminance of the
Table 3. Ratio of the luminance of OLED devices with the YSZ scattering layer to the luminance of
reference OLED without the scattering layer, for various layer thickness.
the reference OLED without the scattering layer, for various layer thickness.
Changed Ratio of
Changed Total
Ratio of Total Changed Ratio of
Changed Normal
Ratio of Normal
Thickness
ThicknessofofScattering
ScatteringLayer
Layer(µm)
(um) Luminance Direction Luminance
Luminance Direction Luminance
0 0(without
(withoutscattering
scatteringlayer)
layer) 100% 100% 100% 100%
1.5
1.5 123% 123% 131% 131%
2.5
2.5 129% 129% 138% 138%
4.0
4.0 126% 126% 135% 135%
7.0 119% 128%
7.0 119% 128%

(a) (b)

Figure5.5.Simulated
Figure Simulatedluminance
luminancechange
changeofofthetheOLED
OLEDdevice
devicewith
withthetheimplemented
implem YSZ scattering layer:
(a)Schematic
(a) Schematicdiagram
diagramand
andparameters
parametersofofthe theOLED
OLEDdevice;
device;(b)
(b)Simulated
Simulatedtotal
totalluminance
luminanceand
andcenter
center
luminancetotonormal
luminance normaldirection
directionasasa afunction
functionofofthe
thethickness
thicknessofofthe
thescattering
scatteringlayer.
layer.

Figure
Figure66illustrates
illustratesthe
therelative
relativeangular
angularluminance
luminancedistribution
distributionofofthe
theOLED
OLEDdevice
devicewith
withthe
the
implemented
implementedYSZ YSZnanoparticle
nanoparticle scattering
scattering layer
layer as
as aafunction
function of
ofthickness
thickness of
ofthe
thescattering
scattering layers.
layers.
Compared to Lambertian distribution, for the reference device it was observed that the luminance at
high angles was larger than that at normal direction. The OLED devices with implemented scattering
layers showed enhanced luminance distribution at all the angles. Moreover, at the scattering layer
thickness of 2.5 um, the most enhanced luminance was achieved. Consequently, the YSZ nanoparticle
scattering layer enhanced the light extraction efficiency to all angular directions by the optimized
Nanomaterials 2019, 9, 1241 7 of 9

Compared to Lambertian distribution, for the reference device it was observed that the luminance at
high angles was larger than that at normal direction. The OLED devices with implemented scattering
layers showed enhanced luminance distribution at all the angles. Moreover, at the scattering layer
thickness of 2.5 µm, the most enhanced luminance was achieved. Consequently, the YSZ nanoparticle
scattering layer enhanced the light extraction efficiency to all angular directions by the optimized
scatter effect. Moreover, enhanced light extraction at high viewing angles improved the angular
color change of the OLED device. As Figure 7 shows, the white angular dependency (WAD), which
represents color change by angular viewing direction, decreased significantly. The color coordinate
Nanomaterials 2019, 9, 1241 7 of 9
change (∆u’v’)
Nanomaterials of the
2019, reference device at 60◦ was 0.028, while that of the OLED device with the 72.5
9, 1241 of µm
9
thick scattering layer was 0.005, which is an 82% decrease of color change. Hence,
um thick scattering layer was 0.005, which is an 82% decrease of color change. Hence, due to the due to the scatter
umofthick
effect
scatterthe scattering
YSZ
effect layer
ofnanoparticle
the YSZ was 0.005,scattering
scattering
nanoparticle which is layer,
layer, we an 82% wedecrease
achieved ofnot
not only
achieved color
onlychange.
enhanced light Hence,
enhanced lightdue
extraction to the
efficiency
extraction
scatter effect of the YSZ nanoparticle scattering layer, we achieved not only enhanced light extraction
butefficiency but alsoangular
also improved improved angular
color change color change
of the OLEDof the OLED device.
device.
efficiency but also improved angular color change of the OLED device.

Figure 6. Relative angular luminance distribution of OLED devices with the implemented YSZ
Figure 6. 6.Relative
Figure Relativeangular
angular luminance distribution of OLED
OLED devices
deviceswith
withthe
theimplemented
implemented YSZ
nanoparticle scattering layerluminance
versus thedistribution
thickness ofofscattering layers, compared YSZ
to the reference
nanoparticle scattering
nanoparticle layer versus
scatteringdistribution.the
layer versusThe thickness of
theLambertian scattering
thickness of layers, compared
scatteringislayers, to the reference device
device and Lambertian distribution plottedcompared to the
using scale-up to reference
the same
and Lambertian
device and distribution.
Lambertian The Lambertian
distribution. The distribution
Lambertian is plotted
distribution is usingusing
plotted scale-up to the
scale-up tosame value
the same
value of reference device at 0 degree for relative comparision.
of reference device at 0 degree for relative comparision.
value of reference device at 0 degree for relative comparision.

Figure Change
7. 7.
Figure Changeofofcolor
colorcoordinates
coordinates(∆u’v’)
(Δu’v’) of
of the OLED device
the OLED devicewith
withthe
theimplemented
implemented2.52.5
um µm thick
thick
YSZFigure 7. Change
nanoparticle of color
scattering coordinates
layer (Δu’v’)
versus the of the
viewing OLED device
angle.
YSZ nanoparticle scattering layer versus the viewing angle. with the implemented 2.5 um thick
YSZ nanoparticle scattering layer versus the viewing angle.
4. Conclusions
4. Conclusions
The implemented YSZ nanoparticle material and planarization material endured, without
The implemented
deformation, YSZ thermal
the subsequent nanoparticle material
annealing andatplanarization
process material
the temperature rangedendured,
to 580 °C.without
Highly
deformation, the subsequent thermal annealing process at the temperature ranged to 580 °C.process
efficient OLED devices can be manufactured using the conventional display manufacturing Highly
efficient OLED devices can be manufactured using the conventional display manufacturing process
Nanomaterials 2019, 9, 1241 8 of 9

4. Conclusions
The implemented YSZ nanoparticle material and planarization material endured, without
deformation, the subsequent thermal annealing process at the temperature ranged to 580 ◦ C. Highly
efficient OLED devices can be manufactured using the conventional display manufacturing process by
implementing YSZ nanoparticles. A 38% enhancement in luminance of the OLED device was achieved
by the scattering layer with a thickness of 2.5 µm, compared to the device without the scattering layer.
Moreover, the decreased angular color change was obtained by implementation of the nanoparticle
scattering layer, where the white angular dependency (WAD) ∆u’v’ was reduced to 0.005 at 60 degrees
from normal direction. Thus, we believe that this study can provide a simple, practical, and low-cost
method for improving the performance of OLED display products.

Author Contributions: Conceptualization, C.Y.P.; B.C. methodology, C.Y.P. investigation, C.Y.P. writing, C.Y.P.
supervision, B.C. funding acquisition, B.C.
Funding: This research was supported by Industrial Human Resources and Skill Development Program (N0001415,
Display Expert Training Project for Advanced Display equipment and components engineer) funded by the
Ministry of Trade, Industry & Energy (MOTIE, Korea).
Conflicts of Interest: The authors declare no conflict of interest.

References
1. Moon, C.K.; Suzuki, K.; Shizu, K.; Adahi, C.; Kaji, H. Combined Inter- and Intramolecular Charge-Transfer
Processes for Highly Efficient Fluorescent Organic Light-Emitting Diodes with Reduced Triplet Exciton
Quenching. Adv. Mater. 2017, 29, 1606448. [CrossRef] [PubMed]
2. Kühn, M.; Pflumm, C.; Glaser, T.; Harbach, P.; Jaegermann, W.; Mankel, E. Band alignment in organic light
emitting diodes—On the track of thickness dependent onset voltage shifts. Org. Electron. 2017, 41, 79.
3. Uoyama, H.; Goushi, K.; Shizu, K.; Nomura, H.; Adachi, C. Highly efficient organic light-emitting diodes
from delayed fluorescence. Nature 2012, 492, 234. [PubMed]
4. Mac Ciarnain, R.; Michaelis, D.; Wehlus, T.; Rausch, A.F.; Wehrmeister, S.; Schmidt, T.D.; Brütting, W.;
Danz, N.; Bräuer, A.; Tünnermann, A. Plasmonic Purcell effect reveals obliquely ordered phosphorescent
emitters in Organic LEDs. Sci. Rep. 2017, 1826. [CrossRef] [PubMed]
5. Saxena, A.K.; Jain, V.K.; Mehta, D.S. A review on the light extraction techniques in organic electroluminescent
devices. Opt. Mater. 2009, 32, 221. [CrossRef]
6. Hong, K.; Lee, J. Recent developments in light extraction technologies of organic light emitting.
Elect. Mater. Lett. 2009, 7, 77.
7. Gather, M.C.; Reineke, S. Recent advances in light outcoupling from white organic light-emitting diodes.
J. Photonics Energy 2015, 5, 057607. [CrossRef]
8. Cheng, Y.H.; Wu, J.L.; Cheng, C.H. Enhanced light outcoupling in a thin film by texturing meshed.
Appl. Phys. Lett. 2007, 90, 091102.
9. Yamasaki, T.; Sumioka, K.; Tsutsui, T. Organic light-emitting device with an ordered monolayer of silica
microspheres as a scattering. Appl. Phys. Lett. 2000, 76, 1243. [CrossRef]
10. Bathelt, R.; Buchhauser, D.; Gärditz, C.; Paetzold, R.; Wellmann, P. Light extraction from OLEDs for lighting
applications through light scattering. Org. Electron. 2007, 8, 293. [CrossRef]
11. Sun, Y.; Forrest, S.R. Enhanced light out-coupling of organic light-emitting devices using embedded low-index
grids. Nat. Photonics 2008, 2, 483. [CrossRef]
12. Do, Y.R.; Kim, Y.C.; Song, Y.W.; Lee, Y.H. Enhanced light extraction efficiency from organic light emitting
diodes by insertion of a two-dimensional photonic crystal structure. J. Appl. Phys. 2004, 96, 7629. [CrossRef]
13. Lee, Y.J.; Kim, S.H.; Huh, J.; Kim, G.H.; Lee, Y.H. A high-extraction-efficiency nanopatterned organic
light-emitting diode. Appl. Phys. Lett. 2003, 82, 37.
14. Lin, L.; Shia, T.K.; Chiu, C.J. Silicon-processed plastic micropyramids for brightness enhancement applications.
J. Micromech. Microeng. 2000, 10, 395. [CrossRef]
15. Moller, S.; Forrest, S.R. Improved light out-coupling in organic light emitting diodes employing ordered
microlens arrays. J. Appl. Phys. 2002, 91, 3324. [CrossRef]
Nanomaterials 2019, 9, 1241 9 of 9

16. Lin, H.Y.; Ho, Y.H.; Lee, J.H.; Chen, K.Y.; Fang, J.H.; Hsu, S.C.; Wei, M.K.; Lin, H.Y.; Tsi, J.H.; Wu, T.C. Efficiency
improvement and image quality of organic light-emitting display by attaching cylindrical microlens arrays.
Opt. Express 2008, 16, 11044. [CrossRef] [PubMed]
17. Kim, H.S.; Kim, C.K.; Jang, H.W. Fabrication of a microball lens array for OLEDs fabricated using a monolayer
microsphere templat. Electron. Mater. Lett. 2013, 9, 39. [CrossRef]
18. Wei, M.K.; Lee, J.H.; Lin, H.Y.; Ho, Y.H.; Chen, K.Y.; Lin, C.C.; Wu, C.F.; Lin, H.Y.; Tsi, J.H.; Wu, T.C. Efficiency
improvement and spectral shift of an organic light-emitting device by attaching a hexagon-based microlens
array. J. Opt. A Pure Appl. Opt. 2008, 10, 5. [CrossRef]
19. Jin, Y.; Feng, J.; Zhang, X.L.; Bi, Y.G.; Bai, Y.; Chen, L.; Lan, T.; Liu, Y.F.; Chen, Q.D.; Su, H.B. Solving
Efficiency–Stability Tradeoff in Top-Emitting Organic Light-Emitting Devices by Employing Periodically
Corrugated Metallic Cathode. Adv. Mater. 2012, 24, 1187. [CrossRef]
20. Kim, D.; Ha, J.; Park, J.; Hwang, J.; Jeon, H.; Lee, C.; Hong, Y. Enhanced light outcoupling of polymer
light-emitting diodes with a solution-processed, -flattening photonic-crystal underlayer. J. Inf. Disp. 2016, 17,
143. [CrossRef]
21. Park, W.Y.; Kwon, Y.; Lee, C.; Whang, K.W. Light outcoupling enhancement from top-emitting organic
light-emitting diodes made on a nano-sized stochastic texture surface. Opt. Express 2014, 22, A1687.
[CrossRef] [PubMed]
22. Park, W.Y.; Kwon, Y.; Cheong, H.W.; Lee, C.; Whang, K.W. Increased light extraction efficiency from
top-emitting organic light-emitting diodes employing a mask-free plasma-etched stochastic polymer surface.
J. Appl. Phys. 2016, 119, 095502. [CrossRef]
23. Gu, X.; Qiu, T.; Zhang, W.; Chu, P.K. Light-emitting diodes enhanced by localized surface plasmon resonance.
Nanoscale Res. Lett. 2011, 6, 199. [CrossRef] [PubMed]
24. Jung, M.; Yoon, D.M.; Kim, M.; Kim, C.; Lee, T.; Kim, J.H.; Lee, S.; Lim, S.H.; Woo, D. Enhancement of hole
injection and electroluminescence by ordered Ag nanodot array on indium tin oxide anode in organic light
emitting diode. Appl. Phys. Lett. 2014, 105, 013306. [CrossRef]
25. Song, H.J.; Han, J.; Lee, G.; Sohn, J.; Kwon, Y.; Choi, M.; Lee, C. Enhanced light out-coupling in OLED
employing thermal-assisted, self-aggregated silver nano particles. Org. Electron. 2018, 52, 230. [CrossRef]
26. Hwang, M.; Kim, C.; Choi, H.; Chae, H.; Cho, S.M. Light extraction from surface plasmon polaritons and
substrate/waveguide modes in organic light-emitting devices with silver-nanomesh electrodes. Opt. Express
2016, 24, 29483–29495. [CrossRef]
27. Xu, L.H.; Ou, Q.D.; Li, Y.Q.; Zhang, Y.B.; Zhao, X.D.; Xiang, H.Y.; Chen, J.D.; Zhou, L.; Lee, S.T.; Tang, J.X.
Microcavity-Free Broadband Light Outcoupling Enhancement in Flexible Organic Light-Emitting Diodes with
Nanostructured Transparent Metal–Dielectric Composite Electrodes. ACS Nano 2016, 10, 1625. [CrossRef]

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