Organic Electronics 14 (2013) 20392045

Contents lists available at SciVerse ScienceDirect

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

Organic/metal hybrid cathode for transparent organic

light-emitting diodes
Jin Woo Huh 1, Jaehyun Moon 1, Joo Won Lee, Jonghee Lee, Doo-Hee Cho, Jin-Wook Shin,
Jun-Han Han, Joohyun Hwang, Chul Woong Joo, Jeong-Ik Lee , Hye Yong Chu
OLED Research Center, Electronics and Telecommunications Research Institute, Daejeon 305-700, Republic of Korea

a r t i c l e

i n f o

Article history:
Received 23 October 2012
Received in revised form 31 March 2013
Accepted 16 April 2013
Available online 9 May 2013
Keywords:
Transparent organic light-emitting diodes
Organic/metal hybrid cathode
Cs-doped electron transport layer (Cs-ETL)/
Ag
Microstructure

a b s t r a c t
We report a highly transparent organic/metal hybrid cathode of a Cs-doped electron transport layer (Cs-ETL)/Ag for transparent organic light-emitting diode (TOLED) applications.
Particular attention is paid to the surface morphology on the Ag lm and its inuence on
the optical transparency and electrical conductivity. With the use of Cs-ETL, a smooth
and continuous surface morphology of Ag lm was achieved, leading to a high transmittance of 75% in TOLED with a low sheet resistance of 4.5 X/Sq in cathode lm. We successfully applied our Cs-ETL/Ag transparent cathode to fabricate highly transparent
OLEDs. Our approach suggests a new electrode structure for transparent OLED applications.
2013 Elsevier B.V. All rights reserved.

1. Introduction
A transparent organic light-emitting diode (TOLED) refers to an OLED type which emits light from the top and
bottom directions of the device [1,2]. In the absence of applied voltage, the TOLED is a transparent window, but
when voltage is applied to the TOLED, it becomes is a bidirectional light-emitting device. Thus, a TOLED can be
used as a light source for innovative window-like lighting
luminaire systems: during the daytime, a TOLED can be
used as an ordinary window, while after sunset the TOLED
can serve as a lighting facility. Because the generated light
in a TOLED has to escape the top surface as well as the bottom surface, special attention has to be paid to the top
electrode, which is the cathode [35].
In conventional bottom-emission OLEDs, the cathode
material is usually metallic with a thickness of approximately 200 nm. Hence, the cathode surface, which is in
contact with the organic layer, acts as a mirror and reects
Corresponding author. Tel.: +82 42 860 1166; fax: +82 42 860 1029.
1

E-mail address: jiklee@etri.re.kr (J.-I. Lee).

First co-author (equal contribution).

1566-1199/$ - see front matter 2013 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.orgel.2013.04.035

the generated light toward direction of the bottom, contributing to the intensity of the bottom emission. On the
other hand, in TOLEDs, in addition to the electrical conductivity, the cathode must have optical transparency. Regarding the electrical conductivity in an electrode, metallic
materials offer sufciently low resistance. However, due
to their absorption dependency on the thickness, a limitation exists when seeking to obtain both high transmittance
and low resistance.
To realize practical TOLEDs, the transmittance of the device initially has to be improved. Therefore, a metal cathode is the key part to improve the transmittance of OLED
devices [6,7]. Conventionally, LiF/Al/Ag has been used as
a transparent cathode [79]. But, in this structure, the
emission intensity may be lowered due to the absorption
loss in the cathode. To make matters worse, with cavity
glass seal [10] of the cathode, a TOLED with a LiF/Al/Ag
cathode gives transmittance of only 60% at 550 nm because
light loss of approximately 10% occurs at the glass cap
boundary due to difference in refractive indices. For higher
transparency, it is crucial to minimize the absorption and
to make the metal lm as thin as possible. Hence, the Al
layer in a conventional transparent cathode of LiF/Al/Ag

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J.W. Huh et al. / Organic Electronics 14 (2013) 20392045

should be removed because it has high absorption in the

visible light region. Moreover, for an effective electron
injection from the Ag layer, modication of the electron
injection layer (EIL) corresponding to LiF should follow.
According to previous several reports, in order to enhance
electron injection in OLEDs, Cs2CO3 has been used as an ntype dopant [1113]. Compared to pristine ETL thin lms,
Cs2CO3 doped organic ETL showed enhanced electron
injection and transport properties [11,14,15]. In addition,
compared to reactive metals as n-type dopants, the incorporation of Cs2CO3 can effectively eliminate diffusion of
metal atoms into the underlying organic layer and consequential nonradiative recombination [11].
In this work, we present an approach which is useful for
reducing the detrimental absorption effect without sacricing the electrical conductance. To be specic, we have
replaced the LiF/Al under the metal (Ag) cathode by a Csdoped organic ETL. First, we removed the Al layer because
the Al layer is the main cause of absorption loss. Thus, LiF/
Al layer was then replaced by an organic electron transport
layer (ETL). However, removing Al layer did not improve
the optical transmittance in actual measurement and its
optical simulations alone could not explain the observed
results of our work. Thus, we investigated the surface
microstructure of the cathode lm. Thermally deposited
organic ETL lms can offer surface smoothness and optical
transparency. In addition, with Cs2CO3 addition, enhanced
electrical properties are expected. Therefore, with an
objectivity of obtaining a smooth Ag lm surface morphology which is favored in transmittance and conductivity, we
have replaced the LiF/Al lm by an organic ETL. In our discussion, we emphasize the importance of the microstructure in analyzing and improving both transmittance and
electrical conductivity.
In this study, we investigated the surface morphologyproperty relationship of the cathode and offered a very
important yardstick in designing transparent electrodes.
Finally, we demonstrated full functionality of TOLEDs having a cathode structure of Cs-ETL/Ag.
2. Experimental
The TOLED has the following stacking sequence: indium
tin oxide (ITO) (70 nm)/TAPC (55 nm)/TCTA: Firpic (7%)
(5 nm)/DCzPPy:Firpic (10%) (5 nm)/BmPyPB (15 nm)/cathode/TAPC (60 nm). The organic material of each layer is
listed in Table 1.
In the rst part of the experiment, we investigated the
thickness effect of the Al layer, which is a part of the cathode, on the transmittance of TOLEDs. The cathode structure

is LiF (1 nm)/Al (X nm)/Ag (15 nm), which is formed on the

ETL of BmPyPB (40 nm). The Al thickness was varied, at
either 0 or 1.5 nm. Previously, in an effort to enhance the
transmittance of TOLEDs, we added a capping layer (CL)
of TAPC onto the cathode surface [16]. Using optical simulations, we investigated the transmittance of TOLEDs as a
function of the CL thickness. The highest transmittance
was obtained at a CL thickness of 60 nm. Based on this result, we xed the CL thickness at 60 nm in this work.
In the second part of the experiment, we replaced the
LiF/Al part in the LiF/Al/Ag structure with a Cs-doped ETL
(Cs-ETL). Thus, the TOLED cathode has the structure of
Cs-ETL (40 nm)/Ag (15 nm). Cs2CO3 was co-evaporated
with ETL and the doping level was varied, at 0, 10, 20 or
40%. Using a TOLED device with the Cs-ETL structure, we
obtained the Cs doping concentration which yields the
highest transmittance.
In the nal part, we demonstrated a fully functional
TOLED with a Cs-ETL/Ag cathode. Its transmittance, EL
spectrum, and current density (J)voltage (V)luminance
(L) characteristics were compared to those of a TOLED with
a LiF/Al/Ag cathode.
The fabrication processes were described in our previous work [17]. All organic and metallic layers were deposited by thermal evaporation in a high vacuum chamber
below 6.7  105 Pa. The fabricated OLEDs were encapsulated with a glass cap. In this course, a glass cap with cavity
was glued using a UV curable resin. Also a moisture getter
was placed inside the cavity glass. The electroluminescence spectrum was measured using a Minolta CS-1000.
The currentvoltage (IV) and luminescence-voltage (L
V) characteristics were measured with a current/voltage
source/measure unit (Keithley 238) and a Minolta CS100. Transmittance of the glass-cap encapsulated TOLED
was measured using an UVvisible spectrophotometer
(U-3501, Hitachi). The surface morphologies of the cathode
lms were investigated by means of scanning electron
microscopy (SEM, Model: Sirion 400, Philips) and atomic
force microscopy (AFM, Model: Park System, XE-100).
Sheet resistance was measured using four-point probe system ((CMT-series, CHANG MIN CO., Ltd.) The simulations
were performed using an OLED optical simulator, SimOLED [18,19] to optimize the characteristics of transparent OLEDs as a function of the thickness of the TAPC.
Briey, the program has inputs of the refractive index
and thickness of every layer. The program employs thin
lm optics and the dipole emission model to calculate
the optical and spectral characteristic of OLEDs. In order
to obtain realistic simulation results, we used all of the
measured optical constants (n, k) of organic materials, as

Table 1
The full name of organics and their functions.
Abbreviation

Chemical name

Function

TAPC

1,1-bis[(di-4-tolylamino)phenyl]cyclohexane

TCTA
Firpic
DCzPPy
BmPyPB

4,40 ,400 -tris(N-carbazolyl)-triphenylamine

0
Iridium(III)bis(4,6-diuorophenyl)-pyridinato-N,C2 )picolinate
2,6-bis(3-(carbazol-9-yl)phenyl)pyridine
1,3-bis(3,5-di-pyrid-3-yl-phenyl)benzene

Hole transport layer

Capping layer
Emitter host
Emitter dopant (blue)
Emitter host
Electron transport layer

J.W. Huh et al. / Organic Electronics 14 (2013) 20392045

obtained using an ellipsometer (M-2000d, J.A. Woollam

Co.).
3. Results and discussion
3.1. Preliminary studies on the Al insert
In TOLEDs, a transparent cathode of LiF/Al/Ag structure
is frequently used [79]. The sheet resistance is expected
to decrease further as the thickness of the Al insert increases. In terms of the electrical performance of the device, increasing the thickness of the Al insert can lower
the operation voltage condition of the OLED devices. However, in terms of the transmittance, increasing the Al thickness is not desirable. The BeerLambert law dictates an
exponential decrease in the transmittance upon an increase in the lm thickness. Thus, a thicker Al layer has
lower transmittance. In this scheme, the transmittance of
LiF/Al/Ag is expected to decrease as the thickness of the
Al insert increases.
Fig. 1 compares the simulated and measured transmittances of the LiF/Al/Ag structure. Here, the thicknesses of
the LiF and Ag are xed at 1 nm and 15 nm. The thickness
of Al (tAl) was varied, at 0 nm or 1.5 nm. In the simulations,
as expected, the insertion of Al lowers the transmittance in
the entire visible wavelength range. However, in the experiments, the insertion of Al does not necessarily lower the
transmittance in the entire visible wavelength range.
To understand this result, we investigated the surface
morphology of the Ag lm. In thin-lm optical simulations,
the optical parameters of the refractive index (n) and
extinction coefcient (k) as well as the thin lm thickness
of the media are considered as the main variables, whereas
the actual microstructures of the thin lms are not.
Fig. 2 shows the two SEM surface images of 15-nm
thick Ag lms which reside on LiF (Fig. 2a) and on an Al

2041

layer (Fig. 2b), respectively. In both cases, the Ag lms

are granular, but the grain sizes of Ag on LiF are much
smaller with more rough surface; The average grain size
of the Ag lm on LiF is 25 nm which is less about a
tenth of that of Ag lm on Al, and root-mean square
(rms) roughness is 15 nm while Ag lm on Al has
2 nm. As described earlier, granular and rough Ag lms
with less than 20 nm in thickness experience light loss
due to surface plasmon resonance (SPR) [2022] as well
as grain boundary scattering [23]. It is noticeable that
SPR-induced loss increases considerably with rms roughness of the lm [20] while the scattering no longer occurs
to any signicant extent when the size of the grain
boundary of the lms is below the size of the wavelength
of the light being scattered. From this, we expect that
more rough granular surface of the Ag lm on LiF experiences larger transmittance loss than that of Ag lm on Al
by SPR-induced absorption rather than scattering. This
supports the result showing that the transmittance of
LiF/Ag is lower than LiF/Al/Ag, as shown in Fig. 1.
The surface morphology in Fig. 2 also explains the
changes in the electrical conductance of the Ag lms. The
initial stage of metallic lm growth is governed by the Volmer-Weber mechanism [24]. At the beginning of lm
growth, separate islands initially form after the deposition
of metal. Next, when the number of islands increases, the
individual islands start to connect physically. The lm becomes continuous only when a certain thickness is
reached, which corresponds to the percolation thickness.
The percolation thickness is dependent on the material
system. In Fig. 2, one can deduce that the percolation thickness of Ag on LiF is much thicker than that of Ag on Al. In
the case of Ag on LiF, the Ag granules are not only small
(25 nm) but are also rarely connected. Meanwhile, Ag
on Al shows much larger granules, which are mainly physically connected.

Fig. 1. Simulated and measured transmittances of LiF/Al/Ag. tAl refers to the Al thickness. (Transmittance was measured under glass reference.)

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J.W. Huh et al. / Organic Electronics 14 (2013) 20392045

Fig. 2. Surface SEM images of (a) LiF/Ag (15 nm) and (b) LiF/Al (1.5 nm)/Ag (15 nm).

The surface energy difference can be used for a rough

comparison of the percolation thickness of an identical
metallic lm on a different type of support. If the surface
energy of the support is lower than the deposited lm,
there exists a driving force that exposes the surface of
the support, which results in restraining the formation of
the percolation network. In this context, a system which
has a larger value of dg i=j ! Dci=j is expected to have a
thicker percolation thickness. Here, dg i=j ! Dci=j is the surface energy difference between i (deposit) and j (support).
The reported surface energies of LiF, Al and Ag are 0.34 J/
m2, 1.1 J/m2, and 1.3 J/m2, respectively [25]. The
dg Ag=LiF ! DcAg=LiF and dg Ag=Al ! DcAg=Al values are 0.96 J/
m2 and 0.2 J/m2, respectiv/ely. Thus, the percolation thickness of Ag on LiF is thicker than that of Ag on Al. In our
material systems, it is apparent that the Al insert has the
effect of thinning the percolation thickness of the deposited Ag. The difference in the percolation thickness can
be examined by measuring the sheet resistance. The measured sheet resistance of LiF/Al/Ag was 7 W=sq ! X=sq.
The sheet resistance of LiF/Ag was approximately
107 W=sq ! X=sq, which is too high for OLED applications. This reects the fact that percolation is established
in Ag on Al, implying a thinner percolation thickness of
Ag on an Al support.
To sum up, in a TOLED with a cathode of LiF/Al/Ag, the
Al contributes by making the Ag lm continuous and facilitates the formation of percolation paths. As a result, compared to the Ag in the LiF case, higher transmittance and
lower sheet resistance were achieved. The former is due
to the reduced scattering and the latter is due to the high
density of the percolation paths.
3.2. Organic lm as an Al replacement
In this section, we probe the possibility of replacing the
Al insert with an organic material. Compared to metallic
thin lms, organic thin lms bear lower optical absorption.
For the purpose of eliminating the Al layer, we also removed the LiF as well because LiF is known to work almost
exclusively with Al [14,26]. As mentioned before, we
choose a Cs-doped ETL (Cs-ETL) as a replacement for Al.

Thus, the new cathode structure is Cs-ETL/Ag (15 nm). In

the current work, we focus on achieving not only high optical transmittance but also low cathode sheet resistance.
Regarding this task, we investigated both as a function of
the Cs concentration, as controlled by adjusting the relative the deposition amounts of the ETL and Cs.
The Fig. 3b(1) shows surface images of Ag lms on undoped and Cs-doped ETL. With undoped ETL, Ag lm on
undoped ETL shows granular features with more high density of grain boundaries. As Cs is doped, signicant grain
growth can be observed. Larger grains and less boundaries
are observed in Ag lms. Such distinct difference in the
surface morphology strongly indicates that the Cs addition
is modifying the ETL surface to induce high wettability of
Ag on the Cs-ETL. It is thought that Cs addition modies
the surface energy of the ETL to make Ag wetting more
favorable. Based on the results of Figs. 1 and 2, this modied surface morphology due to high wettability in Cs-ETL/
Ag gives the result of improvement in transmittance and
electrical conductance.
Optical and electrical properties of the Ag lm were
shown in Fig. 3a. The sheet resistance decreases with a relatively steep slope just after Cs-doping. The reduced sheet
resistance by Cs-doping is associated with enhanced conduction owing to the increased carrier concentration as
well as modied microstructure. But then it saturates to
4.5 X/sq at Cs concentration higher than 10%. Also, the
transmittance increases up to 20% Cs and then decreases
slightly as the Cs concentration increases. The transmittance is still around 60% in the Cs concentration range
of 1040%. Referring to the SEM images above results,
these observations indicate that the Ag surface smoothening effect of Cs addition has a certain upper bound.
Fig. 3b(2) shows the nk products from measured n and k
of Ag lms which reside on undoped and Cs 20% doped
ETL. The Cs-doped sample exhibits lower nk product. Because the amount of absorption is proportional to nk, this
result indicates a decrease in the transmittance loss due
to relatively low absorption in Ag on the Cs-ETL system.
However, the measured nk values are only apparent values.
The apparent change in nk values should be attributed as a
microstructure induced effect. In other words, optics alone

J.W. Huh et al. / Organic Electronics 14 (2013) 20392045

2043

Fig. 3. (a) Transmittance and sheet resistance of the Cs-ETL/Ag(15 nm) lm as a function of Cs concentration (Transmittance was measured under air
reference and evaluated by averaging in the wavelength range of 400700 nm.). (b-1) Surface SEM images of Cs-ETL/Ag lms depending on Cs
concentration. (b-2) nk product and (b-3) transmittance of two Cs-ETL/Ag lms, both undoped or Cs 20% doped, in the visible wavelength range.

can only explain the transmittance change in terms of nk,

which is misleading without the description of the microstructure. From the result of Fig. 3a, we chose a Cs concentration of 20%, which results in a highest transmittance and
low sheet resistance of 63% and 4.5 X/sq, respectively.
Regarding the quality of the transparent conductive lms,
one may use a gure of merit, which is dened as r/a
[27]. Here r and a are the electrical conductivity and the
visible absorption coefcient, respectively. The r/a is obtained using the relations of {Rs ln(T + R)}1, in which Rs
is the sheet resistance in ohms per square, T and R is the
total visible transmittance and reectance, respectively.
As it shows, a larger value of r/a indicates better performance of the transparent electrodes. The r/a values of
our Cs-undoped and doped(20%) ETL/Ag lms are 0.7
and 1.2, respectively, which show Cs-doped (20%) ETL/Ag
lms have better opto-electrical performance than that of
undoped ETL/Ag lms and is comparable to that of lm
of doped-ZnO.
Fig. 4a shows the surface roughness of the Ag lms on a
Cs (20%)-ETL and on LiF/Al according to SEM results as
shown in Fig. 4b. As mentioned previously, the SEM images
show that the Ag lm on the Cs-ETL is almost featureless,
whereas the morphology of the Ag lm on Al is granular.
The AFM scan diagrams revealed that the peak-to-peak
roughness of Ag lms on the Cs-ETL does not exceed
3 nm, while that on LiF/Al exceed 11 nm. The surface morphology of Ag on the Cs-ETL is not only smoother but also
more continuous. Such a feature indicates the high wettability of Ag on the Cs-ETL, which leads to an improvement
in the transmittance due to both less scattering- and less
SPR-induced light loss as well as lower sheet resistance
due to the dense percolation paths in the Ag lm on the
Cs-ETL, as mentioned above. The rms roughness values of
Ag lms on a Cs-ETL and on LiF/Al were found to be

0.6 nm and 1.9 nm, while the sheet resistances were

4.5 X/Sq and 7 X/Sq, respectively.
3.3. TOLED with a Cs-ETL/Ag cathode
Fig. 5 demonstrates a TOLED bearing our new cathode
structure of Cs-ETL/Ag. The gure shows the transmittance
(Fig. 5a), EL spectra (Fig. 5b) and the JVL relationship
(Fig. 5c and d) of TOLEDs with an Ag cathode on the
Cs(20%)-ETL and LiF/Al structures. Fig. 5a shows that the
transmittance of the TOLED with the Cs-ETL/Ag cathode
is higher than that of the TOLED with the LiF/Al/Ag cathode
without a change in the overall transmittance curve shapes
throughout the visible wavelength range. The Cs-ETL/Ag
cathode led to an improvement of up to 20% in the visible
wavelength range. Transmittance of over 70% was achieved
at 550 nm by means of conventional glass encapsulation.
The inset of Fig. 5a shows an actual image of our TOLED
with the Cs-ETL/Ag cathode. The institutional logo is
clearly observable. Fig. 5b shows that replacing LiF/Al with
a Cs-ETL does not induce any change in the EL spectra of
the bottom and top side emissions. These results imply
that replacing LiF/Al with an organic ETL introduces an
enhancement of the transmittance without any signicant
change in the internal optics of the TOLED.
Fig. 5c and d compare the JV and LV characteristics of
two TOLEDs with different cathode structures. In the JV
plot, the two samples exhibit current levels that are nearly
identical to the applied voltage. The LV plot shows that
the TOLED with the Cs-ETL/Ag structure shows an
improvement in the luminance of the top emission. This
improvement in the top side is thought to have its origin
in the higher transmittance in the top cathode of the CsETL/Ag structure, as shown in Fig. 5a. Similar JV characteristics or better LV characteristics imply that the OLED

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J.W. Huh et al. / Organic Electronics 14 (2013) 20392045

Fig. 4. (a) The AFM line-scan across the Ag lms on Cs(20%)-ETL and LiF/Al (The deep points in the AFM scan diagram LiF/Al/Ag represent the open granular
border regions.). (b) The Ag lm morphology on (a) Cs(20%)-ETL and LiF/Al.

Fig. 5. (a) The transmittances, (b) EL spectra and (c) JV (d) LV characteristics of TOLEDs with Cs(20%)-ETL/Ag or LiF/Al/Ag cathodes. (Transmittance was
measured under air reference. Inset in (a) is the photograph of the institutional logo through the TOLED device.)

structure used in the TOLED with the LiF/Al/Ag cathode is

applicable to a TOLED with a Cs-ETL/Ag cathode, which
also implies that the Cs-ETL/Ag cathode structure is feasi-

ble for use in highly efcient TOLEDs. The technical importance of Figs. 4 and 5 is that the replacement of Al with a
Cs-ETL makes the Ag surface smoother and more

J.W. Huh et al. / Organic Electronics 14 (2013) 20392045

continuous, which then improves the optical transmittance and electrical characteristics of the TOLED.
From these results, we found that an improvement of
the optical and electrical properties can be achieved by
applying the Cs-ETL/Ag cathode structure. This indicates
that our organic/metal hybrid cathode structure is a potential candidate as a cathode in efcient transparent OLEDs.
4. Conclusion
Designing a highly transparent cathode is of prime
importance in transparent OLED applications. For this reason, we designed a new organic/metal hybrid cathode with
a Cs-ETL/Ag layer to obtain highly transparent efcient
TOLEDs. In a conventional LiF/Al/Ag transparent cathode,
the Al induces the formation of highly granular Ag lms,
which can potentially deteriorate the optical transmittance
and sheet resistance. By replacing the LiF/Al with an organic ETL layer, it is possible to obtain a smooth continuous Ag
surface morphology, which plays a signicant part in
reducing the light loss due to scattering and SPR, and
enhancing the transmission. By doping Cs into the ETL,
compared to LiF/Al/Ag cathode TOLEDs, better LV characteristics are obtained. Also, identical EL spectra are obtained. In terms of TOLED processing, our cathode design
is highly attractive because it obviates the need to modify
the OLED stack structure. Our approach for an organic/metal transparent electrode may form the basis of highly efcient TOLED applications.
Acknowledgements
This work was supported by IT R&D program of MOTIE/
KEIT, Rep. of Korea (KI002068, Development of Eco-Emotional OLED Flat-Panel Lighting) and ICT R&D program
2013 of MSIP (Ministry of science ICT & Future Panning)
(10041416, Development of Light and Space Adaptable
Display).
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