Christian Eickhoff, Peter Murer, Thomas Geßner, Jan Birnstock, Michael Kröger, Zungsun Choi, Soichi Watanabe, Falk May, Christian Lennartz, Ilona Stengel, Ingo Münster, Klaus Kahle, Gerhard Wagenblast, Hannah Mangold
KEYWORDS: Organic light emitting diodes, Electron transport, Excitons, External quantum efficiency, Polymethylmethacrylate, Luminescence, Fluorescence resonance energy transfer, Diodes, Energy efficiency, Energy transfer
In this paper, two OLED device concepts are introduced. First, classical phosphorescent green carbene emitters with unsurpassed lifetime, combined with low voltage and high efficiency are presented and the associated optimized OLED stacks are explained. Second, a path towards highly efficient, long-lived deep blue systems is shown. The high efficiencies can be reached by having the charge-recombination on the phosphorescent carbene emitter while at the same time short emissive lifetimes are realized by fast energy transfer to the fluorescent emitter, which eventually allows for higher OLED stability in the deep blue.
Device architectures, materials and performance data are presented showing that carbene type emitters have the potential to outperform established phosphorescent green emitters both in terms of lifetime and efficiency. The specific class of green emitters under investigation shows distinctly larger electron affinities (2.1 to 2.5 eV) and ionization potentials (5.6 to 5.8 eV) as compared to the "standard" emitter Ir(ppy)3 (5.0/1.6 eV). This difference in energy levels requires an adopted OLED design, in particular with respect to emitter hosts and blocking layers. Consequently, in the diode setup presented here, the emitter species is electron transporting or electron trapping.
For said green carbene emitters, the typical peak wavelength is 525 nm yielding CIE color coordinates of (x = 0.33, y = 0.62). Device data of green OLEDs are shown with EQEs of 26 %. Driving voltage at 1000 cd/m2 is below 3 V. In an optimized stack, a device lifetime of LT95 > 15,000 h (1000 cd/m2) has been reached, thus fulfilling AMOLED display requirements.
Apart from usage of organic light emitting diodes for flat panel display applications OLEDs are a potential candidate for
the next solid state lighting technology. One key parameter is the development of high efficient, stable white devices. To
realize this goal there are different concepts. Especially by using highly efficient phosphorescent guest molecules doped
into a suitable host material high efficiency values can be obtained. We started our investigations with a single dopant
and extended this to a two phosphorescent emitter approach leading to a device with a high power efficiency of more
than 25 lm/W @ 1000 cd/m2. The disadvantage of full phosphorescent device setups is that esp. blue phosphorescent
emitters show an insufficient long-term stability. A possibility to overcome this problem is the usage of more stable
fluorescent blue dopants, whereas, due to the fact that only singlet excitons can decay radiatively, the efficiency is lower.
With a concept, proposed by Sun et al.1 in 2006, it is possible to manage the recombination zone and thus the
contribution from the different dopants. With this approach stable white color coordinates with sufficient current
efficiency values have been achieved.
One of the unique selling propositions of OLEDs is their potential to realize highly transparent devices over the
visible spectrum. This is because organic semiconductors provide a large Stokes-Shift and low intrinsic absorption
losses. Hence, new areas of applications for displays and ambient lighting become accessible, for instance, the
integration of OLEDs into the windshield or the ceiling of automobiles. The main challenge in the realization of
fully transparent devices is the deposition of the top electrode. ITO is commonly used as transparent bottom
anode in a conventional OLED. To obtain uniform light emission over the entire viewing angle and a low series
resistance, a TCO such as ITO is desirable as top contact as well. However, sputter deposition of ITO on top of
organic layers causes damage induced by high energetic particles and UV radiation. We have found an efficient
process to protect the organic layers against the ITO rf magnetron deposition process of ITO for an inverted
OLED (IOLED). The inverted structure allows the integration of OLEDs in more powerful n-channel transistors
used in active matrix backplanes. Employing the green electrophosphorescent material Ir(ppy)3 lead to IOLED
with a current efficiency of 50 cd/A and power efficiency of 24 lm/W at 100 cd/m2. The average transmittance
exceeds 80 % in the visible region. The on-set voltage for light emission is lower than 3 V. In addition, by vertical
stacking we achieved a very high current efficiency of more than 70 cd/A for transparent IOLED.
Compared to established LCD and plasma technologies displays based on organic light emitting diodes (OLEDs)
promise more brilliant images, less energy consumption and lower production costs. Furthermore, the organic
layers that make up an OLED can be engineered to be transparent in the visible part of the spectrum. In
combination with transparent conductive oxides like Indium-Tin-Oxide (ITO) or Aluminum doped Zinc-Oxide
(AZO) as contacts OLEDs may be built entirely transparent. One major issue to be addressed in the fabrication
of these devices is the deposition of the top transparent contact without damaging the organic layers.
Transparent OLED pixels can be arranged to form entirely transparent OLED displays. For the active matrix
addressing of the individual OLED pixels, we use TFTs which are transparent themselves. Rather than silicon,
they are based on the wide-bandgap semiconductor Zinc-Tin-Oxide (ZTO) and transmit about 80 % of the visible
light (400-750 nm). The transistors typically have field-effect mobilities of 13 cm2/Vs (an order of magnitude
larger than a-Si TFTs) and an on-off ratio of 106. The OLED pixel which needs to be driven may be positioned
directly on top of the driver circuit. The pixels fabricated accordingly have an overall transmittance > 70 %
in the visible spectrum. The brightness of the OLED pixels could be varied from 0 to 700 cd/m2 via the gate
bias of the driving TFTs. These devices state the initial building blocks of future, large-area, high-resolution
transparent OLED displays. More complex transparent driving circuits, required to compensate eventual device
variations will be discussed.
Organic field effect transistors are expected to be applicable for low-cost, large-area electronic applications, e.g. the incorporation as active-matrix into displays based on organic light emitting diodes (OLED). There are two major challenges which have to be tackled. As the low charge carrier mobility allows only for comparatively low saturation currents, the ratio of channel width and length has to increase by several orders of magnitude, compared to poly-Si-technology. Furthermore, as organic semiconductor devices usually degrade upon exposure to solvents, standard photolithography cannot be applied once the organic materials have been deposited. Therefore, the definition of single pixels has to occur before the deposition of organic materials.
We prepared OFETs employing a bottom-Al-gate, an 50 nm thick anodized Al-oxide gate dielectric and a inter-digital drain-source-structure (Au), topped with 30 nm of pentacene as active layer. By applying an inter-digital structure we increased the W/L-ratio to 4340. For the given configuration, a saturation current of 4 mA could be observed at -20 V drain-source- and -20 V gate-source-voltage.
The drain-source-contacts enclosed a predefined ITO-anode shorted to drain and acting as OLED-anode. For preventing shortcuts between the OLED-cathode and the OFET, poly-vinyl-alcohol (PVOH) was spin-coated from an aqueous solution and structurized by photolithography. When the OFET characteristics were measured afterwards the field-effect- mobility dropped by two orders of magnitude but recovered due to desorption of residual water. Afterwards, the organic layers and a Al/LiF-cathode were deposited. The area covered by the OLED was 1.33mm2. Applying an operating bias of 11 V between cathode and source, allows for switching of the OLED by changing the gate-source-voltage from +2.5 V to -5 V. The on-state-brightness is 850 cd/m2 and the on-off-ratio 950. Considering a realistic filling factor of 40% the values observed may be sufficient for active-matrix display-applications.
RGB-OLED-displays can be realized by at least three different approaches: Color from white, color from blue or patterning of red, green and blue OLEDs, which is favorable for reasons of higher efficiency and lower costs. Common patterning techniques like photolithography cannot be applied due to the degradation of the OLEDs after the exposure to solvents. Shadow masking which is currently widely applied is not applicable for bigger substrate sizes of future mass production tools.
Therefore a novel approach for patterning of organic semiconductors will be demonstrated. The laser induced local transfer (LILT) of organic small molecule materials allows for mass production of high resolution RGB-OLED-displays.
An infrared absorbing target is coated with the desired emitting material, which is placed in a short distance in front of an OLED substrate. A scanner deflects and focuses an infrared laser beam onto the target. By adjusting scanning speed and laser power accurately the target locally heats up to a temperature where the organic material sublimes and will be deposited on the opposite OLED substrate. By repeating this for red, green and blue emitting materials a RGB-OLED-display can be realized.
For process evaluation and development a LILT-module has been built, incorporating two custom vacuum chambers, several lift and transfer stages, a high-speed high-precision scanner and an infrared continuous-wave laser (cw). This module is designed to be part of a future inline deposition system for full-color OLED displays. In the first experiments it could be observed, that the pattern resolution is strongly dependent on the scanning speed, exhibiting minimum feature sizes of 40μm. It can be deducted that this is due to the laser's beam profile (TEM00), which allows for the smallest focus possible, but may not allow for rugged process conditions suitable for production. Rectangular steep-edged beam profiles may overcome this problem.
Inverted organic light-emitting diodes showing light emission from
the top are discussed. Top-emitting organic light-emitting diodes
are required for next-generation active-matrix organic
light-emitting displays , as Si-driving circuitry has to be
incorporated into the display itself. We focus on hybrid anodes,
thereby giving a simple model for spin-coating of PEDOT:PSS on top
of an organic layer-stack, LiF-based cathodes and phosphorescent
emitters, allowing for highly efficient inverted organic light
emitting diodes. A maximum current efficiency of 55.4 cd/A at
140 cd/m2 and a maximum luminous efficiency of 17.2 lm/W at
50 cd/m2 has been obtained.
Top-emitting organic light-emitting diodes (OLEDS) fornext-generation active-matrix OLED-displays (AM-OLEDs) arediscussed. The emission of light via the conductive transparent top-contact is considered necessary in terms of integrating OLED-technology to standard Si-based driver circuitry. The inverted OLED configuration (IOLED) in particular allows for the incorporation of more powerful n-channel field-effect transistors preferentially used for driver backplanes in AM-OLED displays. The use of the highly conductive polymer PEDOT:PSS as hole injection layer yields anodes with an extremely low contact resistance. The non-destructive spin-coating is enabled by a hydrophobic buffer layer such as pentacene. The overlying transparent electrode was realized employing low-power radio-frequency magnetron sputter-deposition of indium-tin-oxide (ITO). Additionally, a cathode with an interfacially metal-doped electron-injecting layer is proposed. Hybrid inverted OLEDs utilizing the fluorescent emitter system Alq3:Ph-QAD allowed efficiencies of 2.7 lm/W around 150 cd/m2. Device efficiencies are increased by employing a phosphorescent dye Ir(ppy)3 doped into the hole-transporter TCTA. Such phosphorescent hybrid IOLEDs exhibit peak efficiencies of 19.6 cd/A and 5.8 lm/W at 127 cd/m2. Thus, the main requirements for a use of hybrid inverted IOLEDs in AM-OLED-displays are satisfied.
Top-emitting organic light-emitting diodes (OLEDS) for next-generation active-matrix OLED-displays (AM-OLEDs) are discussed. The emission of light via the conductive transparent top-contact is considered necessary in terms of integrating OLED-technology to standard Si-based driver circuitry. The inverted OLED configuration (IOLED) in particular allows for the incorporation of more powerful n-channel field-effect transistors preferentially used for driver backplanes in AM-OLED displays. To obtain low series resistance the overlying transparent electrode was realized employing low-power radio-frequency magnetron sputter-deposition of indium-tin-oxide (ITO). The devices introduce a two-step sputtering sequence to reduce damage incurred by the sputtering process paired with the buffer and hole transporting material pentacene. Systematic optimization of the organic growth sequence focused on device performance characterized by current and luminous efficiencies is conducted. Apart from entirely small-molecule-based IOLED that yield 9.0 cd/A and 1.6 lm/W at 1.000 cd/m2 a new approach involving highly conductive polyethylene dioxythiophene-polystyrene sulfonate (PEDOT:PSS) as anode buffers is presented. Such hybrid IOLEDs show luminance of 1.000 cd/m2 around 10 V at efficiencies of 1.4 lm/W and 4.4 cd/A.
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