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October 1, 2013 / Vol. 38, No.

19 / OPTICS LETTERS

3773

Enhancement of outcoupling efficiency of


organic light-emitting diodes using a
planarized moth-eye structure on glass substrate
Jeong Ho Kim,1 Lee-Mi Do,2 Je-Hong Choi,1 Jaehoon Park,3 and Heon Lee1,*
1

Department of Materials Science and Engineering, Korea University, 5-1 Anam-dong, Sungbuk-gu, Seoul 136-713, South Korea
2

IT Convergence Technology Research Department, ETRI, 218 Gajeong-ro, Yuseong-gu, Deajeon 305-700, South Korea
3

Department of Electronic Engineering, Hallym University, Chuncheon 200-702, South Korea


*Corresponding author: heonlee@korea.ac.kr
Received May 10, 2013; accepted July 19, 2013;
posted August 28, 2013 (Doc. ID 189990); published September 19, 2013

To improve optical properties of organic light-emitting diodes (OLEDs), we developed a planarized moth-eye structure by ultraviolet nanoimprint lithography (UV-NIL). The moth-eye pattern was fabricated on a glass substrate by
UV-NIL using AMONIL polymer resin. It contains nanoscaled, cone-shaped, periodic pattern arrays with a 250 nm
diameter and a 550 nm pitch. The glass substrate with the moth-eye structure exhibited a 1%2% improvement in
transmittance of visible wavelengths, but it requires a planarized layer with high-refractive-index materials. Photosensitive titanium precursor resin annealed by UV was used to improve the current efficiency by up to 26% versus
conventional OLEDs. 2013 Optical Society of America
OCIS codes: (160.6060) Solgel; (230.3670) Light-emitting diodes; (240.0240) Optics at surfaces; (310.6860) Thin films,
optical properties.
http://dx.doi.org/10.1364/OL.38.003773

Organic light-emitting diodes (OLEDs) have been shown


to be a very attractive light source for the future [1,2].
OLEDs are inexpensive and perform efficiently as flat
light sources. Additionally, they can be applied to a flexible surface [3,4]; therefore, it is possible to design them
to be implemented on a variety of substrates. However,
the light extraction efficiency of OLEDs is limited due to
the total internal refraction (TIR) caused by a difference
in the refractive index of each layer [59]. For this reason, various strategies have been employed to improve
the light extraction efficiency of the OLEDs, including
thickness control of OLED layers for the microcavity
effect [10], light amplification by a Bragg mirror [11],
optical band gap control using a photonic crystal [12],
and a variety of nanoscale patterned layers (enhancement of light outcoupling efficiency) [1317]. To fabricate nanoscale patterns with a simple and economic
process, alternative nanopatterning technologies were
developed, such as nanoimprint lithography, holographic
lithography, and nanosphere lithography [1821]. The
moth-eye structure has antireflection properties that
reduce the TIR of light though the gradual change in
the reflective index of the media [22,23].
We report here the fabrication of a moth-eye structure
on a glass substrate between the substrate and a transparent anode, to improve light outcoupling efficiency
of OLEDs. The moth-eye structures are formed by ultraviolet nanoimprint lithography (UV-NIL). Photosensitive
titanium precursor resin is used as a planarized layer [24].
The organic layers are deposited on the planarized motheye structure to fabricate an OLED and its optical properties are measured.
Schematics of the OLED fabrication process with a
moth-eye structure are shown in Fig. 1. A nickel stamp
having a moth-eye structure was used for the imprint
process, which was fabricated using a combination of
holography and Ni electroforming processes. A polydimethylsiloxane (PDMS) mold made from a SYLGARD
0146-9592/13/193773-03$15.00/0

184 silicone elastomer kit (Dow Corning, Inc.) was used


to replicate the moth-eye structure from the Ni master
stamp. The PDMS mold was placed on a glass substrate
and coated by polymer resin (AMONIL), and was then
pressed at 2 bar, while being exposed to UV radiation
for 5 min.
The PDMS mold was slowly detached from the glass
substrate after the resin was cured. Then we fabricated
a nanoscaled moth-eye structure. However, surface patterns make it difficult to fabricate a highly functioning
OLED using this glass substrate. If organic layers are deposited onto this glass substrate, the OLED does not
work well due to a very high sheet resistance. Therefore,
we used titanium di-n-butoxide bis(2-ethylhexanoate) to
form a planarization layer on the moth-eye structure. Titanium di-n-butoxide bis(2-ethylhexanoate) was dissolved in hexane to reduce viscosity, spin-coated at
1500 rpm for 20 s, and then baked on a hot plate at
60C for 3 min to remove residual solvent in the film.
In order to cure the resin, the film was exposed to UV
for about 10 min (approximately 77 mWcm2 with a

Fig. 1. (a)(d) Fabrication process of moth-eye structure on a


glass substrate, (e) OLED on that substrate, and (f) conventional
OLED.
2013 Optical Society of America

3774

OPTICS LETTERS / Vol. 38, No. 19 / October 1, 2013

major wavelength peak of 365 nm) without any thermal


treatment. Then, an aluminum-doped zinc oxide (AZO)
film was deposited by sputtering. In order to deposit
the organic and aluminum metal layers, the glass substrate was cleaned by immersing in an acetone bath
under sonication for 10 min, followed by immersion in
a methanol bath under sonication for 10 min; then it
was rinsed with deionized (DI) water for 10 min. The
glass substrate was dried under a stream of nitrogen
gas and baked on a hot plate at 120C for 10 min.
The finished OLED structure was as follows: AZO
(70 nm)/NPB (70 nm)/Coumarin 6 (1.0 wt. %) doped in
Alq 3 30 nmAlq 3 (30 nm)/Bphen (40 nm)/LiF (1 nm)/
Al (100 nm). The AZO transparent electrode was deposited by sputtering and the organic layers underwent a
thermal evaporation process.
To achieve the antireflection effect, we fabricated a
moth-eye structure on the glass substrate using the
UV-NIL process shown in Fig. 2(a). The size and pitch
of the pattern were 250 and 550 nm, respectively. Fabricating an OLED using a glass substrate with the moth-eye
structure requires a planarization process before the
transparent electrode is deposited on substrate; otherwise, the sheet resistance of electrode will be greatly increased due to surface roughness. Planarization was
accomplished using a TiO2 solgel process, and the planarized substrate is shown in Fig. 2(b).
The transmittance of the glass substrate with and without a planarized moth-eye structure was measured with
respect to normal incident light in the visible range to analyze the antireflection properties. Figure 3 shows that

Fig. 4. Current densityvoltage (JV ) characteristics of


conventional OLED and OLED developed in this study.

transmittance of the glass having a moth-eye structure


is enhanced by 1%2%.
The sheet resistance of the AZO electrode deposited
on flat glass and glass having planarized moth-eye structures was 15.85 and 18.79 , respectively. The
slight difference in sheet resistance between the two devices could be negligible in the power consumption
of OLEDs.
Figure 4 shows JV characteristics of conventional
OLED and OLED developed in this study. The electrical
properties of the OLED having moth-eye structure were
almost the same as those of conventional OLED. The outcoupling efficiency of OLED was improved by the glass
with the planarized moth-eye structure. In Fig. 5(a), the
developed OLED having planarized moth-eye structure
was brighter than the conventional OLED at the same
current density. The current efficiency was increased
by up to 26% at 1000 cdm2 .

Fig. 2. SEM images of top (inserts) and cross-sectional views


of (a) glass substrate with moth-eye structure and (b) glass
substrate with the moth-eye structure planarized by TiO2 solgel
solution.

Fig. 3. Transmittance measurements of the glass with and


without TiO2 -planarized glass substrate with the moth-eye
structure.

Fig. 5. (a) Luminance versus current density and (b) current


efficiency versus luminance for conventional OLED and OLED
developed in this study.

October 1, 2013 / Vol. 38, No. 19 / OPTICS LETTERS

3775

by the International Collaborative Research and Development Program (N013500005) funded by the Ministry
of Knowledge Economy.

Fig. 6. Schematics of light extraction for (a) a conventional


OLED and (b) an OLED developed in this study. The red-dashed
arrows represent the light path.

Figure 6(a) shows that, while some of the light generated from a conventional OLED escapes, a noticeable
amount is trapped in the glass substrate or transparent
anode electrode due to TIR caused by different reflective
index between glass substrate and AZO electrode. For
this reason, the outcoupling efficiency of the OLED
was decreased. On the other hand, the light outcoupling
efficiency of developed OLED having planarized motheye structure was improved because the generated photons suppressed at the interface can easily escape the device, as shown in Fig. 6(b) [25].
In conclusion, we have fabricated a moth-eye structure
on a glass substrate using a UV nanoimprint technique.
For the stable deposition of an AZO electrode, the planarization process was performed using TiO2 . The results
showed that the OLEDs with or without planarized
moth-eye structure exhibited similar JV characteristics.
In addition, the transmittance was improved by 1%2%,
with normal incident light in the visible range, due to
the antireflection properties. A design utilizing glass with
the moth-eye structure planarized by TiO2 solgel process
was applied to an OLED, which improved the current
efficiency by up to 26% when compared to a conventional OLED.
This research was supported by Nano-Material Technology Development Program through the National
Research Foundation of Korea (NRF) funded by the
Ministry of Education, Science and Technology
(2012M3A7B4035323). This research was also conducted

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