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.
Measured angular dependent emission patterns for all phosphorescent guest−host systems together with fits and error margins of the extracted orientation parameters (PDF).
We report controllable anisotropic light emission of photons originating from vertically aligned transition dipole moments in spun-cast films of CsPbBr nanocubes. By depositing films of nanocrystals on precoated substrates we can control the packing density and resultant radiation pattern of the emitted photons. We develop a technical framework to calculate the average orientation of light emitters, i.e., the angle between the transition dipole moment vector (TDM) and the substrate. This model is applicable to any emissive material with a known refractive index. Theoretical modeling indicates that oriented emission originates from an anisotropic alignment of the valence band and conduction band edge states on the ionic crystal lattice and demonstrates a general path to model the experimentally less accessible internal electric field of a nanosystem from the photoluminescent anisotropy. The uniquely accessible surface of the perovskite nanoparticles allows for perturbation of the normally isotropic emissive transition. The reported sensitive and tunable TDM orientation and control of emitted light will allow for applications of perovskite nanocrystals in a wide range of photonic technologies inaccessible to traditional light emitters.
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