Multiple donor-acceptor design for highly luminescent and stable thermally activated delayed fluorescence emitters.

A considerable variety of donor-acceptor (D-A) combinations offers the potential for realizing highly efficient thermally activated delayed fluorescence (TADF) materials. Multiple D-A type compounds are one of the promising families of TADF materials in terms of stability as well as efficiencies. However, those emitters are always composed of carbazole-based donors despite a wide choice of moieties used in linearly linked single D-A molecules. Herein, we developed a multiple D-A type TADF compound with two distinct donor units of 9,10-dihydro-9,9-dimethylacridine (DMAC) and carbazole as the hetero-donor design. The new emitter exhibits high photoluminescence quantum yield (PLQY) in various conditions including polar media blend and high concentrations. Organic light-emitting diodes (OLEDs) showed a reasonably high external quantum efficiency (EQE). In addition, we revealed that the multiple-D-A type molecules showed better photostability than the single D-A type molecules, while the operational stability in OLEDs involves dominant other factors.

Multiple resonance type thermally activated delayed fluorescence by dibenzo [1,4] azaborine derivatives.

We studied the photophysical and electroluminescent (EL) characteristics of a series of azaborine derivatives having a pair of boron and nitrogen aimed at the multi-resonance (MR) effect. The computational study with the STEOM-DLPNO-CCSD method clarified that the combination of a BN ring-fusion and a terminal carbazole enhanced the MR effect and spin-orbit coupling matrix element (SOCME), simultaneously. Also, we clarified that the second triplet excited state (T2) plays an important role in efficient MR-based thermally activated delayed fluorescence (TADF). Furthermore, we obtained a blue-violet OLED with an external EL quantum efficiency (EQE) of 9.1%, implying the presence of a pronounced nonradiative decay path from the lowest triplet excited state (T1).

The Role of Reverse Intersystem Crossing Using a TADF-Type Acceptor Molecule on the Device Stability of Exciplex-Based Organic Light-Emitting Diodes.

Exciplex system exhibiting thermally activated delayed fluorescence (TADF) holds a considerable potential to improve organic light-emitting diode (OLED) performances. However, the operational lifetime of current exciplex-based devices, unfortunately, falls far behind the requirement for commercialization. Herein, rationally choosing a TADF-type electron acceptor molecule is reported as a new strategy to enhance OLEDs' operating lifetime. A comprehensive study of the exciplex system containing 9,9',9''-triphenyl-9H,9'H,9''H-3,3':6',3''-tercarbazole (Tris-PCz) and triazine (TRZ) derivatives clarifies the relationship between unwanted carrier recombination on acceptor molecules, TADF property of acceptors, and the device degradation event. By employing a proposed "exciton recycling" strategy, a threefold increased operational lifetime can be achieved while still maintaining high-performance OLED properties. In particular, a stable blue OLED that employs this strategy is successfully demonstrated. This research provides an important step for exciplex-based devices toward the significant improvement of operational stability.