Three triazatruxene-based donors Tr-Me, Tr-Ph, and Tr-Tol were intermixed with three acceptors 3P-T2T, 3P-T2P, and 3P-Pyr equipping with different heteroarene cores to generate an array of nine blends to probe the feasibility of exciplex formation.
In this study, a new triazatruxene-based donor Tr-iBu bearing branched alkyl groups is reported to suppress the aggregation found in a previously reported methyl-substituted counterpart Tr-Me. The effects of a steric factor on the propensity of exciplex formation were examined by respectively mixing these triazatruxene-based donors with PO-T2T and two new acceptors PO-T2P and PO-Pyr, all bearing phosphine oxide as the peripheral groups and N-heteroarene cores with different numbers of nitrogen. Based on the steric hindrance of side groups and their corresponding molecular orbitals alignments of donors and acceptors, the characteristics of exciplex-forming systems were analyzed. Among them, the exciplex-forming blends Tr-iBu:PO-T2P and Tr-iBu:PO-Pyr were selected to serve as the emitting layer (EML) to achieve OLED devices with a moderate maximum external quantum efficiency (EQE max ) of 8.27 and 7.54%, respectively. Adopting the Förster resonance energy transfer strategy, the exciplex cohost was doped with a fluorescence emitter, DPy2CN, to realize a deep-red OLED device with the emission peak centered at 674 nm while retaining EQE max of 6.28%. Our results highlight the importance of suppressing the donor aggregation, adequate donor: acceptor combination, and a suitable triplet state of composing the materials for giving efficient exciplex-based OLEDs.
The carbazole of a model compound CPTBF was replaced by αand β-carboline to give donors α-CPTBF and β-CPTBF, respectively. The introduction of carboline leads the new donors to have deeper highest occupied molecular orbital (HOMO) energy levels. Different electron acceptors were tested, among them, a new acceptor, 3,4-CN, was found to give exciplexes with efficient green emissions that are blue-shifted as compared to that of model CPTBF:3,4-CN system. The exciplex formations of α-CPTBF:3,4-CN and β-CPTBF:3,4-CN blends were verified with the significantly red-shifted emissions different from those of constituent donor and acceptor together with the delayed fluorescent observed by time-resolved PL decay experiments. The organic light-emitting diode (OLED) devices with α-CPTBF:3,4-CN and β-CPTBF:3,4-CN blends as the emitting layer showed a maximum external quantum (EQE) of 7.57 and 7.34%, respectively, which is higher as compared to that (EQE = 6.87%) of the model device employing CPTBF:3,4-CN. These results were attributed to the higher exciplex photoluminescence quantum yields due to the higher delay fluorescence components, deeper HOMO, and higher triplet energy of the carboline donors. In addition, the β-CPTBF:3,4-CN exciplex-based OLED exhibited better efficiency roll-off at higher luminesce due to more charge balance with less polaron formation, which was analyzed with time-resolved EL.
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