Highly Efficient Multi‐Resonance Thermally Activated Delayed Fluorescence Material with a Narrow Full Width at Half‐Maximum of 0.14 eV

Multi-resonance thermally activated delayed fluorescence (MR-TADF) material, which possesses the ability to achieve narrowband emission in organic light-emitting diodes (OLEDs), is of significant importance for wide color gamut and high-resolution display applications. To date, MR-TADF material with narrow full width at half-maximum (FWHM) below 0.14 eV still remains a great challenge. Herein, through peripheral protection of MR framework by phenyl derivatives, four efficient narrowband MR-TADF emitters are successfully designed and synthesized. The introduction of peripheral phenyl-based moieties via a single bond significantly suppresses the high-frequency stretching vibrations and reduces the reorganization energies, accordingly deriving the resulting molecules with small FWMH values around 20 nm/0.11 eV and fast radiative decay rates exceeding 108 s-1 . The corresponding green OLED based on TPh-BN realizes excellent performance with the maximum external quantum efficiency (EQE) up to 28.9% without utilizing any sensitizing host and a relatively narrow FWHM of 0.14 eV (28 nm), which is smaller than the reported green MR-TADF molecules in current literatures. Especially, the devices show significantly reduced efficiency roll-off and relatively long operational lifetimes among the sensitizer-free MR-TADF devices. These results clearly indicate the promise of this design strategy for highly efficient OLEDs with ultra-high color purity.