Silylene-Copper-Amide Emitters: From Thermally Activated Delayed Fluorescence to Dual Emission

Angew Chem Int Ed Engl. 2024 Dec 2;63(49):e202410792. doi: 10.1002/anie.202410792. Epub 2024 Oct 16.

Abstract

Herein, we report the inaugural instance of N-heterocyclic silylene (NHSi)-coordinated copper amide emitters (2-5). These complexes exhibit thermally activated delayed fluorescence (TADF) and singlet-triplet dual emission in anaerobic conditions. The NHSi-Cu-diphenylamide (2) complex demonstrates TADF with a very small ΔEST gap (0.01 eV), an absolute quantum yield of 11 %, a radiative rate of 2.55×105 s-1, and a short τTADF of 0.45 μs in the solid state. The dual emissive complexes (3-5) achieve an absolute quantum yield of up to 20 % in the solid state with a kISC rate of 1.82×108 s-1 and exhibit room temperature phosphorescence (RTP) with lifetimes up to 9 ms. The gradual decrease in the intensity of the triplet state of complex 3 under controlled oxygen exposure demonstrates its potential for future oxygen-sensing applications. Complexes 2 and 3 have been further utilized to fabricate converted LEDs, paving the way for future OLED production using newly synthesized NHSi-Cu-amides.

Keywords: Coinage metal complexes; Dual emission; N-Heterocyclic silylene (NHSi); Silylene-copper-amide; Thermally activated delayed fluorescence (TADF).

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