Blue thermally activated delayed fluorescence emitters incorporating acridan analogues with heavy group 14 elements for high-efficiency doped and non-doped OLEDs

Deep-blue thermally activated delayed fluorescence (TADF) emitters are promising alternatives for conventional fluorescence and phosphorescence materials for practical application in organic light-emitting diodes (OLEDs). However, as appropriate bipolar hosts for deep-blue TADF-OLEDs are scarce, the development of efficient deep-blue TADF emitters that are applicable to both doped and non-doped systems is an urgent task. In this study, we developed a new family of blue TADF emitters that demonstrated high photoluminescence (PL) and electroluminescence (EL) quantum efficiencies in both doped and non-doped (neat) systems. Four new donor-acceptor (D-A)-type TADF molecules incorporating phenazasiline, phenazagermine, and tetramethylcarbazole as weak D units and phenothiaborin as a weak A unit were designed and synthesized. By varying the structural rigidity/flexibility as well as the electron-donating ability of the D units, the resulting photophysical and TADF properties of the D-A molecules could be systematically regulated. A comprehensive photophysical investigation revealed that phenazasiline and phenazagermine-based emitters concurrently exhibit blue TADF emissions (464-483 nm), high PL quantum efficiencies (∼100%), extremely fast spin-converting reverse intersystem crossing rates (>10⁷ s^-1), and suppressed concentration quenching. These fascinating features in conjunction produced high-performance doped and non-doped blue TADF-OLEDs. The doped and non-doped TADF-OLEDs using the phenazasiline-based emitter demonstrated extremely high maximum external EL quantum efficiencies (η_ext) of 27.6% and 20.9%, with CIE chromaticity coordinates of (0.14, 0.26) and (0.14, 0.20), respectively. Further, ultra-low efficiency roll-off behavior for both the doped and non-doped devices was demonstrated by their η_ext as high as 26.1% and 18.2%, respectively, measured at a practically high luminance of 1000 cd m^-2