Klemens Brunner

This paper reports an analysis of the properties of polymer light‐emitting devices (PLEDs) doped with iridium complexes. Devices based on charged and neutral complexes doped into poly(vinylcarbazole) (PVK) are presented, and the role of the ions and the charge‐transport properties of the complexes are discussed. In devices with the charged complexes, the concentration of the complex is found to have a profound effect on both the switch‐on voltage and the efficiency. At higher doping concentrations the efficiency is increased and the switch‐on voltage decreased. The increase in efficiency and decrease in switch‐on voltage at higher dopant concentration are found to be due to an alternative charge transport path via the iridium dopant [Ir(bpy)]⁺ (bis(2‐phenylpyridine‐C²,N′)(2,2′‐bipyridine)iridium hexafluorophosphate). However, at lower concentrations the complex becomes an electron trap and the efficiency is reduced. The devices are found to be significantly less efficient than those with neutral complexes. This difference is attributed to the ionic content and the charge trapping properties of the charged complexes. The low efficiency of the charged‐complex‐based devices could be overcome by utilizing a hole‐blocking layer; devices with efficiencies as high as 23 cd A^–1 were obtained.

A series of novel carbazole compounds was synthesized and tested for their suitability as host for triplet emitters in an organic-light emitting diode (OLED). In these compounds, a carbazole unit is either connected to other carbazole units to form carbazole dimers and trimers or to fluorene and oxadiazole derivatives to form mixed compounds. The HOMO level of carbazole compounds can be tuned by substitution at the 3, 6, and/or 9 positions. Making oligomers by connecting carbazole molecules via their 3 (3‘) positions shifts the HOMO level to higher energy, while replacing alkyl groups at the 9 (9‘) positions by aryl groups shifts the HOMO level to lower energy. Furthermore, it has been found that the triplet energy of these compounds is determined by the presence of poly(p-phenyl) chains in the molecular structure. By identifying the longest poly(p-phenyl) chain, one can predict whether a compound will be a suitable host for a high-energy triplet emitter. An overview of HOMO levels, singlet and triplet levels, and exchange energies is given for all carbazole compounds synthesized. Finally, OLEDs employing two selected carbazole compounds as host and fac-tris(2-phenylpyridine)-iridium (Ir(ppy)₃) as guest were constructed and characterized electrically.

The light generating mechanism of a series of light emitting diodes with electron donor–bridge–acceptor systems (D–b–A) as the emitting species was examined by constructing model diodes based on small organic molecules (OLEDs) as well as on molecularly doped electroactive (poly‐N‐vinylcarbazole, PVK) and insulating (polystyrene, PS) polymers (PLEDs). The direct electrogeneration of an intramolecular charge‐transfer (CT) fluorescence of the donor–bridge–acceptor systems occurred readily in OLED devices with a D–b–A system as the emissive layer. In diodes with PS as the host matrix, hole‐injection and electron‐injection occurred directly in the D–b–A molecules residing close to the anode and the cathode, respectively. In the PVK diodes, hole‐injection occurred primarily into PVK and the positive charge carrier was subsequently trapped on the D–b–A molecule, whereas electron‐injection at the cathode side occurred directly into the D–b–A molecules. Charge‐hopping between neighboring molecules then occurred until a hole and electron resided on the same molecule, which is equivalent to the formation of the CT excited state, and which finally relaxed by intramolecular charge recombination under the emission of CT fluorescence.

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