Spirobifluorene-fused strategy enables pure-green multiple resonance emitters with low efficiency roll-off.

Herein, we present a molecular design strategy centered on the spiroannulation of the MR-core skeleton to fabricate green MR-emitters and reduce device efficiency roll-off. Fusing 9,9'-spirobifluorene into the central framework of MR-emitters facilitates the distribution of the highest occupied molecular orbital (HOMO) across the spiro units, leading to a red-shifted emission and giving rise to a pure-green MR-emitter (DPhCz-SFBN) with the Commission Internationale de l'Eclairage (CIE) coordinates of [0.16, 0.74] in toluene solution, closely matching the BT.2020 standard for green. Additionally, the resultant highly twisted hetero[6]helicene conformation and a nearly perpendicular conformation of spirocycle structure effectively minimize close π-π stacking interactions among the MR-emitting cores, thereby reducing exciton quenching. Consequently, organic light-emitting diodes (OLEDs) based on DPhCz-SFBN exhibit a high maximum quantum efficiency (EQE max ) of 32.8% with low efficiency roll-off, maintaining an EQE of 23.2% at a practical luminance level of 5000 cd m -2 .