Adjusting Nitrogen Atom Orientations of Pyridine Ring in Tetraphenylsilane-Based Hosts for Highly Efficient Blue Phosphorescent Organic Light-Emitting Devices

Four wide bandgap host materials, namely, 9-(4-diphenyl(4-(pyridin-3-yl)phenyl)silyl-phenyl)-9H-carbazole (CSmP), 9-(4-diphenyl(4-(pyridin-2-yl)phenyl)silylphenyl)-9H-carbazole (CSoP), 9-(4-diphenyl(4-(pyridin-3-yl)phenyl)silylphenyl)-9H-3,9′-bicarbazole (DCSmP), and 9-(4-(diphenyl(4-(pyridin-2-yl)phenyl)silyl)phenyl)-9H-3,9′-bicarbazole (DCSoP), have developed by incorporation of pyridine with varied N atom orientation and carbazole/dimer carbazole units into the tetraphenylsilane skeleton for blue phosphorescent light-emitting diodes. These host materials all possess wide bandgap (3.54–3.64 eV) and high triplet energies (2.77–2.95 eV). As revealed by the absorption and emission spectra, theoretical calculations, and CV measurements, the N atom orientation exerts a strong influence on the LUMO energy level and electron-transportation behaviors without deterioring the photophysical properties. Among them, DCSmP with 3-pyridyl substituent manifests the best electron-transporting capability. The FIrpic-doped blue phosphorescent device using DCSmP as host material exhibits excellent electroluminescence performance with a maximum current efficiency of 40.1 cd A–1 and a maximum external quantum efficiency of 20.0%. The current efficiency and external quantum efficiency are improved 3-fold, higher than those fabricated from DCSpP with 4-pyridyl as substituent, demonstrating an effective strategy for large improvement in device performance by a subtle change in molecular structure.