Crafting 1,4-diaryl spirobifluorene hosts in OLEDs interannular C-H arylation: synergistic effects of molecular linearity and orthogonality.

In this work, we present a design concept of introducing linear structures into the orthogonal configuration of 9,9'-spirobifluorene (SBF), aiming to enhance carrier mobilities while maintaining high triplet energies ( ), which are two critical parameters for optimizing host materials in organic light-emitting diodes (OLEDs). To validate our proposed design, four pivotal model molecules of 1,4-diaryl SBFs were synthesized interannular C-H arylation of bi(hetero)aryl-2-formaldehydes, a task challenging to accomplish using previous synthetic methodologies. The orthogonal configuration and the steric hindrance of SBF lead to high through the conjugation breaking at C1 and C4 positions, rendering 1,4-diaryl SBFs suitable as universal pure hydrocarbon (PHC) hosts for red, green, and blue (RGB) phosphorescent OLEDs (PhOLEDs). Meanwhile, the linearity and relatively good planarity of the -quaterphenyl structure promote high carrier mobilities through orderly intermolecular packing. The synergistic effects of linearity and orthogonality in 1-(-biphenyl)-4-phenyl-SBF result in exceptional device performance with external quantum efficiencies (EQEs) of 26.0%, 26.1%, and 22.5% for RGB PhOLEDs, respectively. Notably, the green PhOLED exhibits minimal efficiency roll-off, positioning its device performances among the state-of-the-art in PHC hosts.