Acceleration of singlet-triplet intersystem crossings (ISC) is instrumental in bolstering triplet exciton harvesting of multi-resonance thermally activated delayed fluorescent (MR-TADF) emitters. This work describes a simple gold(I) coordination strategy to enhance the spin-orbit coupling of green and blue BN(O)-based MR-TADF emitters, which results in a notable increase in rate constants of the spectroscopically observed ISC process to 3 × 10 9 s À 1 with nearly unitary ISC quantum yields. Accordingly, the resultant thermally-stable Au I emitters attained large values of delayed fluorescence radiative rate constant up to 1.3 × 10 5 /1.7 × 10 5 s À 1 in THF/PMMA film while preserving narrowband emissions (FWHM = 30-37 nm) and high emission quantum yields (ca. 0.9). The vapor-deposited ultrapure-green OLEDs fabricated with these Au I emitters delivered high luminance of up to 2.53 × 10 5 cd m À 2 as well as external quantum efficiencies of up to 30.3 % with roll-offs as low as 0.8 % and long device lifetimes (LT 60 ) of 1210 h at 1000 cd m À 2 .
Acceleration of singlet‐triplet intersystem crossings (ISC) is instrumental in bolstering triplet exciton harvesting of multi‐resonance thermally activated delayed fluorescent (MR‐TADF) emitters. This work describes a simple gold(I) coordination strategy to enhance the spin‐orbit coupling of green and blue BN(O)‐based MR‐TADF emitters, which results in a notable increase in rate constants of the spectroscopically observed ISC process to 3×109 s−1 with nearly unitary ISC quantum yields. Accordingly, the resultant thermally‐stable AuI emitters attained large values of delayed fluorescence radiative rate constant up to 1.3×105/1.7×105 s−1 in THF/PMMA film while preserving narrowband emissions (FWHM=30–37 nm) and high emission quantum yields (ca. 0.9). The vapor‐deposited ultrapure‐green OLEDs fabricated with these AuI emitters delivered high luminance of up to 2.53×105 cd m−2 as well as external quantum efficiencies of up to 30.3 % with roll‐offs as low as 0.8 % and long device lifetimes (LT60) of 1210 h at 1000 cd m−2.
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