High-efficiency blue thermally activated delayed fluorescence from donor-acceptor-donor systems via the through-space...

The photophysical optimization of donor (D)-acceptor (A) molecules is a real challenge because of the intrinsic limitation of their charger transfer (CT) excited states. Herein, two D-A-D molecules featuring blue thermally activated delayed fluorescence (TADF) are developed, in which a homoconjugated acceptor 5,10-diphenyl-5,10-dihydrophosphanthrene oxide (DPDPO2A) is incorporated to bridge four carbazolyl or 3,6-di-t-butyl-carbazolyl groups for D-A interaction optimization without immoderate conjugation extension. It is shown that the through-space conjugation effect of DPDPO2A can efficiently enhance intramolecular CT (ICT) and simultaneously facilitate the uniform dispersion of the frontier molecular orbitals (FMO), which remarkably reduces the singlet-triplet splitting energy (ΔE _ST) and increases FMO overlaps for radiation facilitation, resulting in the 4-6 fold increased rate constants of reverse intersystem crossing (RISC) and singlet radiation. The maximum external quantum efficiency beyond 20% and the state-of-the-art efficiency stability from sky-blue TADF OLEDs demonstrate the effectiveness of the "conjugation modulation" strategy for developing high-performance optoelectronic D-A systems.