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Monocyclometalated (C N) Gold(III) Metallacycles: Tunable Emission and Singlet Oxygen (1O2) Generation Properties


Malmberg, Robert; Suter, Dominik; Blacque, Olivier; Venkatesan, Koushik (2021). Monocyclometalated (C N) Gold(III) Metallacycles: Tunable Emission and Singlet Oxygen (1O2) Generation Properties. Chemistry - A European Journal, 27(58):14410-14417.

Abstract

The synthesis, characterization and photoluminescent properties of four cyclometalated (C N)-type gold(III) complexes bearing a bidentate diacetylide ligand, tolan-2,2'-diacetylide (tda), are reported. The complexes exhibit highly tunable excited state properties and show photoluminescence (PL) across the entire visible spectrum from sky-blue (lambda(PL)=493 nm) to red (lambda(PL)=675 nm) with absolute PL quantum yields (PLQY) of up to 75 % in solution, the highest PLQY found for any monocyclometalated Au(III) complex in solution. As a consequence of the use of the strongly rigidifying diacetylide bidentate ligand, a significant increase in the excited state lifetimes (tau(0)=16-258 mu s) was found in solution and in thin films. The complexes showed remarkable singlet oxygen generation in aerated solution with absolute singlet oxygen quantum yield (phi(1 Delta)) values reaching up to 7.5x10(-5) and singlet oxygen lifetimes (tau(1 Delta)(0)) in the range of 66-95 mu s. Furthermore, the radiative and non-radiative rates of singlet oxygen were determined using the phi(1 Delta) and tau(1 Delta)(0) values and correlations are drawn between the formation of singlet oxygen and its interaction with cyclometalated (C N) gold(III) complexes.

Abstract

The synthesis, characterization and photoluminescent properties of four cyclometalated (C N)-type gold(III) complexes bearing a bidentate diacetylide ligand, tolan-2,2'-diacetylide (tda), are reported. The complexes exhibit highly tunable excited state properties and show photoluminescence (PL) across the entire visible spectrum from sky-blue (lambda(PL)=493 nm) to red (lambda(PL)=675 nm) with absolute PL quantum yields (PLQY) of up to 75 % in solution, the highest PLQY found for any monocyclometalated Au(III) complex in solution. As a consequence of the use of the strongly rigidifying diacetylide bidentate ligand, a significant increase in the excited state lifetimes (tau(0)=16-258 mu s) was found in solution and in thin films. The complexes showed remarkable singlet oxygen generation in aerated solution with absolute singlet oxygen quantum yield (phi(1 Delta)) values reaching up to 7.5x10(-5) and singlet oxygen lifetimes (tau(1 Delta)(0)) in the range of 66-95 mu s. Furthermore, the radiative and non-radiative rates of singlet oxygen were determined using the phi(1 Delta) and tau(1 Delta)(0) values and correlations are drawn between the formation of singlet oxygen and its interaction with cyclometalated (C N) gold(III) complexes.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Scopus Subject Areas:Physical Sciences > Catalysis
Physical Sciences > Organic Chemistry
Uncontrolled Keywords:General Chemistry, Catalysis, Organic Chemistry
Language:English
Date:19 October 2021
Deposited On:13 Jan 2022 14:34
Last Modified:14 Jan 2022 21:00
Publisher:Wiley-VCH Verlag
ISSN:0947-6539
OA Status:Closed
Publisher DOI:https://doi.org/10.1002/chem.202102331
Project Information:
  • : FunderSNSF
  • : Grant ID200020_156967
  • : Project TitleNovel Organometallic Complexes and Polymers Based Luminescent Materials
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