Elaboration of the appropriate host materials proved to be not less important for the fabrication of a highly efficient OLED than the design of emitters. In the present work, we show how by simple variation of molecular structure both blue emitters exhibiting delayed fluorescence and ambipolar high triplet energy hosts can be obtained. The compounds with a para-junction revealed higher thermal stability (T up to 480 °C), lower ionization potentials (5.51-5.60 eV), exclusively hole transport, and higher photoluminescence quantum efficiencies (0.90-0.97). Meta-linkage leads to ambipolar charge transport and higher triplet energies (2.82 eV). Introduction of the accepting nitrile groups in the para-position induces intensive delayed fluorescence via a triplet-triplet annihilation up-conversion mechanism. By utilization of the para-substituted derivative as an emitter and the meta-substituted isomer as the host, a deep-blue OLED with the external quantum efficiency of 14.1% was fabricated.
Rather than donor–acceptor dihedral angles, the TADF performance of DMAC–BZN positional isomers is instead controlled by differences in acceptor strength arising from π-system electron density – along with a through-space dipole interaction.
We present a study of two isomeric thermally activated delayed fluorescence (TADF) emitters 9,9'-(sulfonylbis(pyrimidine-5,2-diyl))bis(3,6-di-tert-butyl-9H-carbazole) (pDTCz-DPmS) and 9,9'-(sulfonylbis(pyrazine-5,2-diyl))bis(3,6-di-tert-butyl-9H-carbazole) (pDTCz-DPzS). The use of pyrimidine and pyrazine as bridging units between the electron donor and acceptor moieties is found to be advantageous compared to the phenyl-(pDTCz-DPS) and pyridine-based analogues (pDTCz-3DPyS and pDTCz-2DPyS). Conformational modulation of the donor groups as a function of the bridge results in high photoluminescence quantum yields (FPL > 68%) and small energy gaps between singlet and triplet excited states (ΔEST < 160 meV). OLEDs using pDTCz-DPmS and pDTCz-DPzS as emitters exhibit blue and green electroluminescence, respectively, with higher maximum external quantum efficiencies (EQEmax of 14% and 18%, respectively) and reduced efficiency roll-off as compared to the reference devices using pDTCz-DPS, pDTCz-3DPyS, and pDTCz-2DPyS as the emitters. Our results provide a more complete understanding on the impact of the bridge structure in D-AD TADF systems on the optoelectronic properties of the emitter, and how the balance between color purity and EQE in the devices can be controlled, advancing the design strategies for TADF emitters.
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