Highly Efficient Thermally Activated Delayed Fluorescence Organic Light-Emitting Diodes with Fully Solution-Processed Organic Multilayered Architecture: Impact of Terminal Substitution on Carbazole–Benzophenone Dendrimer and Interfacial Engineering

A series of second-generation carbazole-benzophenone dendrimer substituted by several functional groups at terminal positions (subG2B) was investigated toward a thermally activated delayed fluorescence (TADF) emitter for nondoped emissive layer (EML) application in a solution-processed organic light-emitting diode (OLED). Substitution was found to dramatically alter the photophysical properties of the dendritic TADF emitters. The introduction of tert-butyl and phenyl group endows the subG2Bs with aggregation-induced emission enhancement character by suppression of internal conversion in singlet excited states. In the meantime, the introduction of a methoxy group resulted in aggregation-caused quenching character. The device performance of the OLED, where subG2B neat films were incorporated as nondoped EMLs, was found to be highly enhanced by adopting fully solution-processed organic multilayer architecture in comparison to the devices with a vacuum-deposited electron transporting layer (ETL), achieving a maximum external quantum efficiency of 17.0%. Such improvement was attributable to the improved carrier balance via intermixing at solution-processed EML/ETL interfaces. It was also found that the post-thermal annealing of the OLED at appropriate temperatures could be beneficial to enhance OLED performance by promoting the intermixing EML/ETL interface to some extent. Our findings emphasize the potential utility of dendritic TADF emitters in the solution-processed TADF-OLED and increase the importance to manipulate dendrimer/small molecule interfaces.