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

Tian-Yi LiDaniel G ShlianPeter I DjurovichMark E Thompson
Published in: Chemistry (Weinheim an der Bergstrasse, Germany) (2021)
A luminescent bimetallic AuI complex comprised of N-heterocyclic carbene (NHC) and carbazole (Cz) ligands, that is, (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 analogue, (NHC)AuCz and (NHC')AuCz. A coplanar geometry designed into the tandem complex ensures sufficient electronic coupling between the π-orbitals of the ligands to impart a strong oscillator strength to the singlet intra-ligand charge-transfer (1 ICT) transition. Theoretical modelling indicates that the emissive ICT excited state involves both NHC ligands. The tandem complex gives blue luminescence (λmax =480 nm) with a high photoluminescent quantum yield (ΦPL =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 (ΔEST =50 meV, 400 cm-1 ) consistent with the short TADF lifetime.
Keyphrases
  • energy transfer
  • quantum dots
  • light emitting
  • metal organic framework
  • sensitive detection
  • photodynamic therapy
  • single molecule
  • mass spectrometry
  • electron transfer