Spontaneous orientation polarization (SOP) results in excess charge accumulation at the interfaces within OLEDs. The excess charge accumulation leads to significant exciton-polaron quenching (EPQ) and correlates to the device degradation. While SOP is observed in various OLED materials, the optimized SOP configuration remains not well understood. In this study, we demonstrated the correlations of the interface charge accumulation and device characteristics, particularly focusing on EPQ and device degradation, by the simultaneous measurement technique of displacement current and photoluminescence intensity (DCM-PL).
We demonstrate a method to control charge accumulation at the hetero interfaces of organic light-emitting diodes (OLEDs) using dipolar doping of hole transport layers (HTLs). Dipolar doping enables spontaneous orientation polarization (SOP) even in nonpolar HTLs, and consequently compensates the negative interface charge originating from SOP of the adjacent layer. This concept was applied to tris-(8-hydroxyquinolate) aluminum (Alq3) and tris (2- phenylpyridine)iridium (Ir(ppy)3)-based OLEDs. We confirmed that dipolar doping modifies the density and polarity of the net interface charge and reduces the luminescence loss due to both hole and electron accumulations via exciton polaron quenching.
In this study, we examined the correlations between the accumulated charge density and triplet-polaron quenching (TPQ) using simultaneous measurement of displacement current and photoluminescence intensity. We applied this technique to metal-insulator-semiconductor devices where a model structure of an Ir(ppy)3-based OLED was involved, in order to investigate the contribution of unipolar charge accumulation. This technique allows us to investigate not only the TPQ rate constant but also the detailed charge distribution around the EML that is influenced by SOP. The results suggest that the SOP management is an important issue to optimize the device performance of OLEDs.
Displacement current measurement (DCM) is a simple but powerful tool for exploring charge carrier dynamics in organic semiconductor devices. In the first section, we review the basic concept of DCM and how it detects the charge injection, extraction, accumulation, and trapping behaviors in organic semiconductor devices within a quasistatic regime. Subsequently, we present applications of this technique to investigate the device properties of tris-(8-hydroxyquinolate) aluminum (Alq3)-based organic light-emitting diodes. We observed that light irradiation during device fabrication induces additional negative space charges and charge traps in the Alq3 layer. In addition, the device containing the illuminated Alq3 film exhibits a lower luminous efficiency and shorter lifetime compared to the device fabricated in dark conditions, possibly because of the additional hole accumulation in the illuminated Alq3 film. DCM detects the formation of charge traps in the aged devices, decay of the negative space charge, and increase in hole injection voltage with device aging. The origins of these behaviors can be attributed to orientation polarization and charge traps in Alq3 film.
The carrier behaviors in pentacene based organic field-effect transistor (OFET) were investigated by impedance
spectroscopy measurement (IS). We clearly observed the carrier injection from the electrode and accumulation at the
pentacene/insulator interface. We propose the measurement circuit for IS in transistor operation by using battery source
for drain voltage. In this method, an additional structure where capacitance gradually increases is observed between
injection and accumulation processes. From the comparison this result and the analyzed curve which reflects the
injection properties from the electrode, we conclude that this additional structure originates from the charge sheet
spreading into channel region. This technique enables us to observe the carrier injection to the channel region and
investigate the charge sheet formation from off-state to on-state and vice versa of OFETs.
A giant surface potential (GSP) has been observed on a
tris-(8-hydroxyquinolate) aluminum (Alq3) film deposited on a glass or a metal substrate under dark conditions. However, the effects of a GSP on the device properties of Alq3-based organic light-emitting diodes (OLEDs) has not been considered. In this paper, we report on the effects of ambient light during the fabrication of an Alq3-based OLED on the device properties by displacement current measurement. We found that the light irradiation significantly reduces the density of charge existing at the
4,4'-bis[N-(1-naphthyl)-N-phenylamino]-biphenyl/Alq3 interface and results in the formation of charge traps in the Alq3 layer. Considering the similarities between the GSP and the interfacial charge, they can be attributed to the same origin; the orientaion polarization of Alq3 film.
We examined the driving mechanism of indium-tin oxide (ITO)/4,4-bis[N-(1-naphthyl)-N-phenyl-amino]biphenyl
(α-NPD)/Tris-(8-hydroxiquinolate) aluminum (Alq3)/cathode type organic light-emitting diode (OLED) by using a displacement current measurement (DCM). The DCM enables us to directly calculate the amount of accumulated charge.
There exists a maximum value in the amounts of the blocked holes at α-NPD/Alq3 interface. The maximum value was
about 120 nC/cm2, this value is consistent with the density of the fixed interfacial charge proposed by Brütting et al. By using hole-only device with Au cathode, we also investigated the hole blocking and the subsequent overflow of hole
current beyond the interface. The observed feature can be explained by the hole blocking due to the interfacial charge
rather than by that due to the HOMO mismatch at the interface.
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