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A Luminescent Two-Coordinate Au(I) Bimetallic Complex with a Tandem-Carbene Structure: A Molecular Design for the Enhancement of TADF Radiative Decay Rate.

A luminescent bimetallic Au(I) complex comprised of N -heterocyclic carbene (NHC) and carbazole (Cz) ligands, i.e. (NHC')Au(NHC)AuCz has been synthesized and studied both carbene ligands in the bimetallic complex act as electron acceptors in tandem to increase the energy separation between the ground and excited state, which is higher than those found in either monometallic analog, (NHC)AuCz and (NHC')AuCz.  A coplanar geometry designed into the tandem complex ensures sufficient electronic coupling between the p-orbitals of the ligands to impart a strong oscillator strength to the singlet intraligand charge-transfer ( 1 ICT) transition.  Theoretical modeling indicates that the ICT excited state involves both NHC ligands.  The tandem complex gives blue luminescence (λ max = 480 nm) with a high photoluminescent quantum yield (Φ PL =0.80) with a short decay lifetime (τ = 0.52 μs).  Temperature dependent photophysical studies indicate that emission is via thermally assisted delayed fluorescence (TADF) and give a small singlet-triplet energy difference (Δ E ST = 50 meV, 400 cm -1 ) consistent with the short TADF lifetime.