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Ultra-thin silver/germanium/silver electrode shows excellent optical, electrical and

mechanical properties, and it can be used as transparent cathode and anode for
top-emitting, bottom-emitting and transparent flexible OLEDs.
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Journal of Materials Chemistry C Accepted Manuscript

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Journal of Materials Chemistry C Accepted Manuscript

Silver/germanium/silver: an effective transparent
Cite this: DOI: xxxxxx
electrode for flexible organic light-emitting devices
Shihao Liu, Wenbo Liu, Jing Yu, Wei Zhang, Letian Zhang, Xuemei Wen, Yongming Yin
and Wenfa Xie*
State Key Laboratory on Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin
Received xxxx,
Accepted xxxx University, Changchun, 130012, People’s Republic of China. E-mail: xiewf@jlu.edu.cn

DOI: xxxxxx
Mechanical resilience is important for future organic light-emitting devices (OLEDs) lighting
www.rsc.org/ and displays. A key constraint is the electrode used in OLEDs. Here we demonstrate ultra-thin
silver/germanium/silver (AGA)-based flexible organic light-emitting devices, with comparable
efficiency to their ITO-based counterparts. The fabrication process of AGA electrode is
compatible with that of the OLED, and they show excellent optical, electrical and mechanical
properties. They can be used as transparent cathode and anode for top-emitting, bottom-
emitting and transparent flexible OLEDs.

Introduction reflectivity, the thickness of the Ag film should be reduced.

Organic light-emitting devices (OLEDs) show strong
competitiveness in the future displays and lighting since they
are lighter, thinner and more flexible. Transparent electrode
with good optical, electrical and mechanical properties is an
essential element for OLEDs. Indium tin oxide (ITO), which
has a high transparence and low sheet resistance, is commonly
used as the transparent electrode in OLEDs.1-4 However, there
are still some problems: limited supply of indium, lack of
flexibility, and the complicated fabrication process.5-7 Thin
metal films, metallic oxides, conductive polymers and
nanoscale conductive materials, such as sliver (Ag) thin film,
Ge-doped In2O3 (IGO), Al-doped SiO (Al:SiO), Poly(3,4-
ethylenedioxythiophene)-poly (styrenesulfonate) (PEDOT:PSS),
graphene, carbon nanotubes, metal nanowires and so on,8-16
have drawn extensive attention to be good alternatives to the
common transparent electrode. Nevertheless, they still have the
challenge of realizing high transparence, low sheet resistance,
high flexibility characteristic and process compatibility.
Although, the conductive polymers and nanoscale conductive
materials have the flexible characteristic, they can only be
fabricated through wet process which hinders their application
to top electrode. Additionally, metallic oxide is fragile and lack
of flexibility.
Metal films with high conductivity are flexible, but they are
mostly high reflectivity and low transmittance, which will
induce strong microcavity effect in devices.17 Green OLEDs
with thin Ag film show higher efficiency due to microcavity
effect than ITO-based devices. However, it is difficult to obtain
white OLEDs by using Ag electrode. In order to realize low
Nevertheless, during the fabrication process, sliver atoms
growing on substrate form isolated islands initially and finally
these islands are connected to cover the whole area; therefore, it
forms as non-continuous clusters below a special film thickness,
which is about 15nm.18 However, the 15 nm Ag film still has a
rather high reflection. Although the transparence of the Ag film
could be improved by capping an outcoupling layer, it is
difficult to obtain high transparence and flexible electrode on
substrate by inserting an outcoupling layer between substrate
and Ag film. Cioarec et al. verified that the presence of a 5 nm
germanium (Ge) nucleation layer can affects the Ag growth
mode.19, 20 When Ag atoms deposited on Ge film, a Volmer-
Weber model of Ag growth along with small and dense
nucleation on dots could contribute to the fast coalescence
(critical thickness<1 nm) in the initial step. Eventually, such
process would lead to a smoother surface. We also have
reported a multilayer transparent cathode consisting of 15 nm
Ag, 5 nm Ge and 5 nm Ag, which can obtain angle-stable red,
green, blue and white top-emitting OLEDs by only adopting
corresponding emitters without changing the thickness of
organic layer.21 However, the efficiencies of the devices are
lower than those of the ITO-based devices due to the relative
low transparence of the cathode.
In this paper, we prove that a 1-nm-thick Ge film can also
markedly affect the Ag growth mode. And then, a 10-nm
multilayer transparent electrode consisting of 1 nm Ag, 1nm Ge
and 8 nm Ag (AGA), which can be fabricated by thermal
evaporation process and applied to both transparent anode and
cathode for OLEDs, is demonstrated. The AGA film shows
desired characteristics for transparent electrode: high

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 Page 3 of 7 Journal of Materials Chemistry C
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DOI: 10.1039/C3TC31927J

transparence, low sheet resistance, excellent mechanical
resilience. The AGA-based top-emitting OLEDs (TEOLEDs),
bottom-emitting OLEDs (BOLEDs) and transparent OLEDs
(TOLEDs) on glass and flexible polyethylene terephthalate
(PET) substrates are successfully fabricated, and the
performances of the flexible devices are discussed in detail.
Experimental
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roughness are high to 20.6 Å or 12.9 Å, respectively, doesn’t
form the continuous film. By contrast, the AGA on glass or
PET has tiny RMS roughness: 5.2 Å or 1.8 Å, respectively,
which indicates that they have formed the smooth continuous
films. Besides, small Ag crystalline grains can be observed in
the microscopy image of the AGA on glass. Compared with
AGA on glass, the grain texture is smaller and the grain density

is much higher in AGA on PET, noting that it has a higher

Device fabrication reflectivity and a smother surface.22 Additionally, although the

Journal of Materials Chemistry C Accepted Manuscript

AGA fabricated on Bphen/Liq has high RMS as 3.79 nm, it still
The organic materials used in our experiments are purchased possesses the continuous film which means the feasibility as a
from Luminescence Technology Corporation. All devices are top electrode; and the relatively high RMS is mostly caused by
fabricated on ITO glass substrates or PET flexible substrates. the rough Bphen/Liq layer under the AGA.
The substrates are subjected to a routine cleaning process with
rinsing in Decon 90, deionized water, drying in an oven, and
finally treating in a UV-ozone chamber. The stacked electrode
AGA and all devices are evaporated by thermal evaporating on
the precleaned glass or PET substrates under the high vacuum
(~5×10-4 Pa) without breaking the vacuum. A shadow mask is
used to define the anode and cathode, and to make four 10 mm2
devices on each substrate. All the organic layers are thermally
deposited in a vacuum at a rate of 1-2 Å/s monitored in situ
with the quartz oscillator.

Device characterization
The sheet resistance and transparency are measured with four-
probe resistance analyzer (Four Probe Tech., Ltd.) and
ellipsometer (J. A. Woollam. Co. Inc), respectively. The surface
morphologies of the electrode AGA are analyzed by atom force
microscopy (AFM). Luminance-current-voltage characteristics
of unpackaged devices are measured simultaneously using a
Keithley 2400 Source Meter and a Minolta Luminance Meter
LS-110 in air at room temperature. The spectra of the devices
are measured with Ocean Optics Maya 2000-PRO spectrometer.
Results and discussion

Figure 1 (a) shows the transmission of glass substrate, PET

substrate, Glass/Ag (10 nm), PET/Ag(10 nm), glass/AGA
(GAGA), PET/AGA (PAGA), glass/Bphen (40 nm)/Liq (2
nm)/AGA, glass/AGA/MoO3(40 nm) and PET/AGA/MoO3 (40
nm). As can be seen from the figure, the measured average
transmission of 10-nm on glass or PET substrate is only 32% or
28% in the visible region, respectively. The low transmission of
10-nm Ag can be attributed to the rough surface of non-
continuous Ag layer which causes excitation of the surface
plasmas and light absorption. In addition, it can be also seen
that the average transmission of GAGA is about 58%, while
that of PAGA is 48%; and a light outcoupling layer MoO3 (40
nm) added on top of the AGA layer can increase the average
transmission of GAGA and PAGA to 65% and 50%,
respectively. When the AGA is used as top electrode
(fabricated on the Bphen/Liq), there is not significant change in
transmission. Besides, the transmission of the AGA layer is
relatively even which would be suitable to the design of the
white device. The difference in transmission between PAGA
and GAGA is mostly caused by the different transmittance
between glass and PET substrate. Moreover, the denser grain
with smaller texture of PAGA also plays a part in its lower
transmission in comparison to GAGA.
Fig. 1 (b) shows the AFM topography images of glass
substrate, PET substrate, PET/Ag (10 nm), glass/Ag (10 nm),
PET/AGA, glass/AGA, glass/Bphen (40nm)/Liq (2 nm)/AGA
and glass/Bphen (40nm)/Liq (2 nm). It clearly shows that 10-
nm Ag on glass or PET, of which the root-mean-sheet (RMS)

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Figure 1. (a) the transmission of glass substrate, PET
substrate, glass/Ag (10 nm), PET/Ag (10nm), glass/AGA,
PET/AGA, glass/Bphen (40 nm)/Liq (2 nm)/AGA,
glass/AGA/MoO3(40 nm) and PET/AGA/MoO3(40 nm). (b)
the AFM topography images (1µm×1µm) of glass substrate,
glass/Ag (10 nm), glass/AGA, PET substrate, PET/Ag (10
nm), PET/AGA, glass/Bphen/Liq/AGA and glass/Bphen
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respectively, while that of IBOLED-G is 34.7 cd/A. Seen from
the inset in Fig.3, PBOLED-G, PTEOLED-G and IBOLED-G
own the similar EL spectra with the same main peak at ~520nm.
However, when compared with ITO-based device, spectra of
the AGA-based device appear to be narrowed slightly due to
the weak microcavity effect. For example, the full width at half
maximum of PBOLED-G and PTEOLED-G is 70 nm and 75

/Liq. (c) the variations of sheet resistance of PET/AGA and nm, while that of IBOLED-G is 90 nm. Additionally, after 100
PET/ITO as the bending cycles. R0 is the initial sheet bending cycles, there is no significant change in the

Journal of Materials Chemistry C Accepted Manuscript

resistance and Rs is the sheet resistance after bending. performance of the flexible AGA-based devices, which is
shown in Fig.3 (c). It obviously demonstrated that the AGA
The micro-crystallization characteristic results in that GAGA electrode has excellent mechanical resilience and strong
has a better electrical conductivity than top AGA electrode and adhesiveness with the organic molecular.
PAGA. The sheet resistances of GAGA, AGA fabricated on
Bphen/Liq and PAGA are 26.0, 40.0, and 77.8Ω/sq,
respectively. Moreover, the PAGA exhibits excellent
mechanical resilience as well. It can be seen in Fig. 1 (c), when
the electrodes on PET are bent at a radius of about 8 mm, the
PAGA exhibits almost no visible change in the sheet resistance
as the bending cycles increase, while that of ITO increases
rapidly. It confirms that the AGA possesses an excellent
mechanical resilience and strong adhesion on PET, which is
essential to fabricate high-performance flexible OLEDs.
In order to demonstrate the effectiveness of this electrode,
AGA-based green/white OLEDs on glass and PET substrates
are fabricated. The AGA-based flexible OLEDs on PET
substrate are discussed in detailed. In the flexible OLEDs, the
AGA electrode is used as anode or cathode in BOLED or
TEOLED, and it is used as anode and cathode in TOLED,
which are marked as PBOLED-G, PTEOLED-G, PBOLED-W,
PTEOLED-W and PTOLED-W, respectively. These devices
share similar structure: PET substrate/Anode/MoO3/Di-[4-
(N,N-ditolylamino)-phenyl] cyclohexane (TAPC)/4,4',4''-tris
(carbazol-9-yl)-triphenylamine (TCTA)/Emission Layer
(EML)/4,7-Diphenyl-1,10-phenanthroline (Bphen)/8-Hydroxy-
quinolinolato-lithium (Liq)/Cathode. The EMLs of the green
OLEDs consist of a bipolar host 2,7-bis (diphenylphosphoryl)-
9-[4-(N,N-dipheny-lamino) phenyl]-9-phenylfluorene (POAPF)
doped with10wt% tris(2-phenyl- pyridine) iridium(III)
[Ir(ppy)3]. Additionally, the EMLs of the white devices are
formed by POAPF doped with bis (3,5-difluoro-2-(2-pyridyl)
phenyl-(2-carboxypyridyl) iridium(III) (Firpic) or iridium(III)
bis(4-phenylthieno[3,2-c]pyridinato-N,C2’) acetylacetonate
(PO-01), which could be written as POAPF:10wt% Firpic (12 Figure 2. The whole schematic layer structures of the
nm)/POAPF: 8wt% PO-01 (18 nm). The whole schematic layer fabricated devices.
structures are given in Fig.2. The MoO3 in the top of the white
TEOLEDs is the light outcoupling layer.
Firstly, the AGA-based green devices PBOLED-G and
PTEOLED-G are discussed. For comparison, the ITO-based
green BOLEDs marked as IBOLED-G are fabricated. Except
for the transparent anode, the IBOLED-G owns the identical
structure with PBOLED-G. The current density-voltage-
luminance and current efficiency-luminance characteristics of
green OLEDs based on AGA and ITO electrodes are shown in
Fig. 3. The AGA-based devices exhibit desirable OLED
electronic characteristic, such as the turn-on voltage as small as
2.4 V, which is approximate to the ITO-based devices (2.3 V).
The low turn-on voltage indicates that AGA electrodes can
offer a sufficient carrier injection, leading to low operating
voltage and power consumption. Although there is faintness
difference at current densities, the AGA-based devices exhibit
the current efficiencies which are comparable to those of the
ITO-based devices. The maximum current efficiencies of
PBOLED-G and PTEOLED-G are 26.7 cd/A and 34.3 cd/A,

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luminance characteristics of PBOLED-W and PTEOLED-W,

and the luminance-voltage-current density characteristics of
these two devices are shown in the inset. The maximum current
efficiencies of PBOLED-W and PTEOLED-W are 22.8 cd/A
and 27.6 cd/A, respectively; and the current efficiencies can
still reach 20.8 cd/A and 26.8 cd/A at the brightness of 1000
cd/m2. Besides, both of the PBOLED-W and PTEOLED-W
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exhibit extremely low efficiency roll-off. From the brightness at

maximum current efficiency to high brightness at 5000 cd/m2,

Journal of Materials Chemistry C Accepted Manuscript

the efficiency roll-off is 9% and 15%, respectively. With regard
to the optical property for PBOLED-W and PTEOLED-W,
their emission spectra keep relatively stable with driving
voltages increasing, as shown in Fig. 5 (b) and (c). It can be
clearly seen that, for both devices, the white emission consists
of phosphorescent blue and yellow emission, stemming from
Firpic and PO-01, respectively. As the voltage increases, the
Figure 3. (a) The current density-voltage-luminance, and (b) change in spectra of PBOLED-W and PTEOLED-W is almost
current efficiency-luminance characteristics of AGA-based invisible to naked eye. The CIE coordinates for PBOLED-W
and ITO-based green devices. The inset is normalized EL and PTEOLED-W shift only (-0.016,-0.009), (-0.009, 0.004)
spectra for PBOLED-G, PTEOLED-G and IBOLED-G. (c) from 4 V to 6 V, respectively.
the ratios of current density, luminance, current efficiency
before and after 100 bending cycles at the bending radius of
about 8 mm for PBOLED-G and PTEOLED-G. J0, L0, CE0
represents the current density, luminance, current
efficiency of the devices before bending, respectively, and
the corresponding after bending is JB, LB, CEB.

Spectra for the AGA-based green devices exhibit relatively

angle stability which is essential to flat panel display. Fig. 4
manifests the spectra for PBOLED-G and PTEOLED-G at
different viewing angles. It can be seen that, as viewing angles
increase, no visible variation is observed in the emission spectra
of both devices. The angle-stable characteristic of the AGA-
based devices should be attributed to the low reflectivity of the
AGA transparent electrode which forms less angle-dependent
cavity emission in the devices.

Figure 5. (a) Current efficiency-luminance characteristics of

PBOLED-W and PTEOLED-W and the insets are their
Figure 4. Normalized EL spectra of AGA-based green corresponding luminance-voltage-current density
devices (a) PBOLED-G and (b) PTEOLED-G at different characteristics. (b) ad (c) Normalized EL spectra of
viewing angles. PBOLED-W and PTEOLED-W under different voltages.

Then, the white AGA-based BOLEDs and TEOLEDs are

discussed and further demonstrated the effectiveness of this
AGA electrode. Fig. 5 (a) presents the current efficiency-

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symmetrical emission characteristics at anode and cathode sides.

For example, at the bias voltage of 7.0 V, the luminance from
top/bottom side of PTOLED-W is 3978/3819 cd/m2. The
maximum current efficiency of top and bottom sides for
PTOLED-W are 10.5 cd/A and 10.6cd/A, respectively. The
inconformity of efficiency of the two sides should be attributed
to the tiny differences at brightness. Besides, PTOLED-W
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obtains the maximum total current efficiency 21.1 cd/A at the

bias voltage of 4V.

Journal of Materials Chemistry C Accepted Manuscript

The emission spectra of AGA-based TOLEDs also exhibit
comparative symmetry from cathode and anode sides. The
normalized EL spectra from both sides of PTOLED are shown
in inset of Fig. 7. The differences in the CIE coordinates
between top and bottom sides for PTOLED are only (0.037,
0.025). In comparison to spectra from bottom side, the blue
emission of top side is enhanced slightly. Like the AGA-based
devices above, EL spectra emitting from both sides for AGA-
based TOLEDs also stay relatively stable with the viewing
Figure 6. Normalized EL spectra for (a) PBOLED-W and (b) angle, which is shown in Fig. 8. As the viewing angle changes
PTEOLED-W at the current density of 20 mA/cm2. The from 0o to 60o, the CIE coordinates of top sides for PTOLED
insets are their corresponding photograph. only change (-0.028, -0.018), while those of bottom side are (-
0.044, -0.026). The angle stability of AGA-based TOLEDs also
Furthermore, like the AGA-based green devices, the can be attributed to the transparent anode and cathode adopting
emission spectra of PBOLED-W and PTEOLED-W also own the low reflectivity AGA, which forms less angle-dependent
the comparatively angle-stable viewing characteristic. Fig. 6 cavity emission in the devices.
shows the EL spectra of PBOLED-W and PTEOLED-W under
different viewing angles. As the viewing angle changes from 0o
to 60o, the CIE coordinates of PBOLED-W only change (-0.009,
-0.028), while those of PTEOLED-W are (0.030, 0.004).This
indicates that PBOLED-W and PTEOLED-W exhibit relatively
angle stability, which is due to the less angle-dependent cavity
emission in the devices formed by their corresponding AGA
transparent anode or electrode with the low reflectivity.

Figure 8. EL spectra of PTOLED from both sides at

different viewing angles and the photograph of PTOLED at
the current density of 20 mA/cm2.

Figure 7. (a) Current density-voltage-luminance and (b)
current efficiency-luminance characteristics of AGA-based
white TOLEDs. The insets are the normalized EL spectra of
PTOLED from both sides at the current density of 20
mA/cm2.
Finally, the AGA-based TOLEDs on the PET substrate are
investigated. Fig. 7 shows the current density-voltage-
luminance and current efficiency-luminance characteristics of
both sides for PTOLED-W. As can be seen, there is a balanced
luminance of bi-directional emission in PTOLED-W due to the
Conclusions
In summary, efficient monochromatic and white AGA-based
flexible OLEDs are demonstrated. The AGA-based flexible
TEOLEDs, BOLEDs and TOLEDs show excellent EL
performances and angle-stable characteristics. This work will
provide an efficient, high transmission and excellent
mechanical resilience transparent electrode, applying to both
cathode and anode, for angle-stable flexible OLEDs.
Acknowledgements
This work was supported by the National Natural Science
Foundation of China (Grant Nos. 60937001, 11074096,
61177026), New Century Excellent Talents in University (No.
100446) and the Ministry of Science and Technology of China
(Grant No. 2010CB327701).

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