Organic light‐emitting diodes (OLEDs) are efficient large‐area light sources facing their market entry. Still, the development of stable and more efficient blue emitters and the enhancement of light outcoupling remain challenges for further device improvements. Here, we review the working principles of OLEDs and highlight ongoing efforts to improve their efficiency, in particular by coupling out more light.

The distinct preferential alignment, i.e., horizontal orientation with respect to the substrate plane, of the optical transition dipole moment vectors (TDMVs) of organic dye molecules is of paramount importance for extracting the internally generated power of organic light-emitting diodes (OLEDs) to the outside world. This feature is one of the most promising approaches for the enhancement of the electrical efficacy in stateof-the-art OLEDs, as their internal quantum efficiencies are already close to the ultimate limit. If one can achieve complete horizontal orientation of the TDMVs, it is possible to increase the efficiency by at least 50% because alignment strongly influences the power dissipation into the different optical modes present in such a thin-film device. Thus, this feature of organic light-emitting molecules can lead to advanced performance for future applications. Therefore, we present here a review of recent achievements, ongoing research, and future tasks in this particular area of organic electronics.

Controlling the alignment of the emitting molecules used as dopants in organic light-emitting diodes is an effective strategy to improve the outcoupling efficiency of these devices. To explore the mechanism behind the orientation of dopants in films of organic host materials, we synthesized a coumarin-based ligand that was cyclometalated onto an iridium core to form three phosphorescent heteroleptic molecules, (bppo)2Ir(acac), (bppo)2Ir(ppy) and (ppy)2Ir(bppo) (bppo represents benzopyranopyridinone, ppy represents 2-phenylpyridinate, and acac represents acetylacetonate). Each emitter was doped into a 4,4'-bis(N-carbazolyl)-1,1'-biphenyl host layer, and the resultant orientation of their transition dipole moment vectors was measured by angle-dependent p-polarized photoluminescent emission spectroscopy. In solid films, (bppo)2Ir(acac) is found to have a largely horizontal transition dipole vector orientation relative to the substrate, whereas (ppy)2Ir(bppo) and (bppo)2Ir(ppy) are isotropic. We propose that the inherent asymmetry at the surface of the growing film promotes dopant alignment in these otherwise amorphous films. Modelling the net orientation of the transition dipole moments of these materials yields general design rules for further improving horizontal orientation.

Influence of the direction of spontaneous orientation polarization on the charge injection properties of organic light-emitting diodes

The orientation distribution of the emissive sites in a phosphorescent Organic LED has been measured utilizing two independent optical methods. In contradiction to common expectations we find a clearly non-isotropic, predominantly parallel emitter orientation in the well-known triplet emitting guest-host system of Ir(MDQ)2(acac) blended in an alpha-NPD matrix. This result emphasizes the necessity of more sophisticated assumptions on active emitter properties in quantitative optical OLED analysis, and demonstrates a highly promising approach for OLED efficiency optimization

An organic light‐emitting diode (OLED) with the blue emitter CC2TA showing thermally activated delayed fluorescence (TADF) is presented exhibiting an external quantum efficiency (ηEQE) of 11% ± 1%, which clearly exceeds the classical limit for fluorescent OLEDs. The analysis of the emission layer by angular dependent photoluminescence (PL) measurements shows a very high degree of 92% horizontally oriented transition dipole moments. Excited states lifetime measurements of the prompt fluorescent component under PL excitation yield a radiative quantum efficiency of 55% of the emitting species. Thus, the radiative exciton fraction has to be significantly higher than 25% due to TADF. Performing a simulation based efficiency analysis for the OLED under investigation allows for a quantification of individual contributions to the efficiency increase originating from horizontal emitter orientation and TADF. Remarkably, the strong horizontal emitter orientation leads to a light‐outcoupling efficiency of more than 30%.

Comparing the emissive dipole orientation of two similar phosphorescent green emitter molecules in highly efficient organic light-emitting diodes Applied Physics Letters 101, 253304 (2012);

Most of the commonly used electron transporting materials in organic light-emitting diodes exhibit interfacial polarization resulting from partially aligned permanent dipole moments of the molecules. This property modifies the internal electric field distribution of the device and therefore enables an earlier flat band condition for the hole transporting side, leading to improved charge carrier injection. Recently, this phenomenon was studied with regard to different materials and degradation effects, however, so far the influence of dilution has not been investigated. In this paper we focus on dipolar doping of the hole transporting material 4,4-bis[N-(1-naphthyl)-N-phenylamino]-biphenyl (NPB) with the polar electron transporting material tris-(8-hydroxyquinolate) aluminum (Alq3). Impedance spectroscopy reveals that changes of the hole injection voltage do not scale in a simple linear fashion with the effective thickness of the doped layer. In fact, the measured interfacial polarization reaches a maximum value for a 1:1 blend. Taking the permanent dipole moment of Alq3 into account, an increasing degree of dipole alignment is found for decreasing Alq3 concentration. This observation can be explained by the competition between dipole-dipole interactions leading to dimerization and the driving force for vertical orientation of Alq3 dipoles at the surface of the NPB layer.