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Red‐emitting organic light‐emitting diodes (OLEDs) are important for displays and lighting, with the latter benefiting from solution processable materials, which would enable low embedded energy, scalable fabrication. Herein, the effect of annealing and phase separation on the performance of solution‐processed OLEDs incorporating a light‐emitting layer composed of the exciplex host, m‐MTDATA:OXD‐7, and a red phosphorescent light‐emitting dendrimer, Ir(tDCpq)3, is described. Solution‐processed OLEDs containing an annealed emissive layer with a low dendrimer concentration (2 wt%) are found to have the best performance, which is higher than the device in which the light‐emitting layer is not annealed. The improvement in the performance of the annealed device is ascribed to improved charge mobility within the emissive layer caused by phase separation of the OXD‐7. The OLEDs containing annealed m‐MTDATA:OXD‐7:(2 wt%) Ir(tDCpq)3 have maximum current, power, and external quantum efficiencies of 17.9 cd A−1, 19.4 lm W−1, and 14.8 ± 0.6%, respectively. The fact that the maximum external quantum efficiency (EQE) of 14.8% is larger than that expected based on the photoluminescence quantum yield (PLQY) and the normal out‐coupling efficiency of 20% from a bottom‐emitting device is determined to arise from the different pathways of exciton formation under photoexcitation and charge injection. [ABSTRACT FROM AUTHOR]

Phosphorescent emissive materials in organic light‐emitting diodes (OLEDs) manufactured using evaporation are usually blended with host materials at a concentration of 3–15 wt% to avoid concentration quenching of the luminescence. Here, experimental measurements of hole mobility and photoluminescence are related to the atomic level morphology of films created using atomistic nonequilibrium molecular dynamics simulations mimicking the evaporation process with similar guest concentrations as those used in operational test devices. For blends of fac‐tris[2‐phenylpyridinato‐C2,N]iridium(III) [Ir(ppy)3] in tris(4‐carbazoyl‐9‐ylphenyl)amine (TCTA), it is found that clustering of the Ir(ppy)3 (surface of the molecules within ≈0.4 nm) in the simulated films is directly relatable to the experimentally‐measured hole mobility. Films containing 1–10 wt% of Ir(ppy)3 in TCTA have a mobility of up to two orders of magnitude lower (≈10−6 cm2 V−1 s−1) than the neat TCTA film, which is consistent with the Ir(ppy)3 molecules acting as hole traps due to their smaller ionization potential. Comparison of the simulated film morphologies with the measured photoluminescence properties shows that for luminescence quenching to occur, the Ir(ppy)3 molecules have to have their ligands partially overlapping. Thus, the results show that the effect of guest interactions on charge transport and luminescence are markedly different for OLED light‐emitting layers. [ABSTRACT FROM AUTHOR]