Multiple resonance induced thermally activated delayed fluorescence: effect of chemical modification

Thermally activated delayed fluorescence (TADF) is the internal conversion of triplet excitons into singlet excitons via reverse intersystem crossing (RISC). It improves the efficiency of organic light-emitting diodes (OLED) by enabling the harvesting of nonradiative triplet excitons. Multiple resonance (MR) induced TADF chromophores exhibit an additional advantage of high color purity due to their rigid conformation. However, owing to the strict design rules there is a limited number of known MR-TADF chromophores. For applications in full-color high-resolution OLED displays, it is desirable to extend the variety of available chromophores and their color range. We computationally explore the effect of chemical modification on the properties of the MR-TADF chromophore quinolino[3,2,1-de]acridine-5,9-dione (QAD). QAD derivatives are evaluated based on several metrics: The formation energy is associated with the ease of synthesis; The spatial distribution of the frontier orbitals indicates whether a compound remains an MR-TADF chromophore or turns into a donor–acceptor TADF chromophore; The change of the singlet excitation energy compared to the parent compound corresponds to the change in color; The energy difference between the lowest singlet and triplet states corresponds to the barrier to RISC; The reorganization energy is associated with the color purity. Based on these metrics, QAD-6CN is predicted to be a promising MR-TADF chromophore with a cyan hue. This demonstrates that computer simulations may aid the design of new MR-TADF chromophores by chemical modification.