Nature Research, Nature Communications, 1(13), 2022
DOI: 10.1038/s41467-021-27739-x
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AbstractPolaron-induced exciton quenching in thermally activated delayed fluorescence (TADF)-based organic light-emitting diodes (OLEDs) can lead to external quantum efficiency (EQE) roll-off and device degradation. In this study, singlet-polaron annihilation (SPA) and triplet-polaron annihilation (TPA) were investigated under steady-state conditions and their relative contributions to EQE roll-off were quantified, using experimentally obtained parameters. It is observed that both TPA and SPA can lead to efficiency roll-off in 2,4,5,6-tetra(9H-carbazol-9-yl)isophthalonitrile (4CzIPN) doped OLEDs. Charge imbalance and singlet-triplet annihilation (STA) were found to be the main contributing factors, whereas the device degradation process is mainly dominated by TPA. It is also shown that the impact of electric field-induced exciton dissociation is negligible under the DC operation regime (electric field < 0.5 MV cm−1). Through theoretical simulation, it is demonstrated that improvement to the charge recombination rate may reduce the effect of polaron-induced quenching, and thus significantly decrease the EQE roll-off.