Hybridized local and charge-transfer (HLCT) emitters
have attracted
extensive attention, but the insolubility and severe self-aggregation
tendency restrict their applications in solution-processable organic
light-emitting diodes (OLEDs), particularly deep-blue OLEDs. Herein,
two novel benzoxazole-based solution-processable HLCT emitters (BPCP
and BPCPCHY) are designed and synthesized, in which benzoxazole acts
as an acceptor, carbazole acts as a donor, and hexahydrophthalimido
(HP, with a large intramolecular torsion angle and spatial distortion
characteristics) acts as a bulky modified end-group with weak electron-withdrawing
effects. Both BPCP and BPCPCHY exhibit HLCT characteristics and emit
near ultraviolet in toluene at 404 and 399 nm. Compared to the BPCP,
the BPCPCHY solid shows much better thermal stability (T
g, 187 vs 110 °C), higher oscillator
strengths of the S1-to-S0 transition (0.5346 vs 0.4809), and faster k
r (1.1
× 108
vs 7.5 × 107 s–1) and thus a much higher ΦPL in the neat film. The introduction of HP groups greatly suppresses
the intra-/intermolecular charge-transfer effect and self-aggregation
trends, and the BPCPCHY neat films placed in air for 3 months can
still maintain an excellent amorphous morphology. The solution-processable
deep-blue OLEDs utilizing BPCP and BPCPCHY achieved a CIEy of 0.06 with maximum external quantum efficiency (EQEmax) values of 7.19 and 8.53%, respectively, which are among the best
results of the solution-processable deep-blue OLEDs based on the “hot
exciton” mechanism. All of the above results indicate that
benzoxazole is an excellent acceptor for constructing deep-blue HLCT
materials, and the strategy of introducing HP as a modified end-group
into an HLCT emitter provides a new perspective to develop solution-processable
efficient deep-blue OLEDs with high morphological stability.