Changes in the optical properties of an alkynyldigold(I) complex upon reaction with Cu(I) are associated with a complicated structural change to form an unusual Au4Cu2 cluster with metallophilic interactions as well as pi-alkyne coordination.
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Scissor-like AuCu Cluster with Phosphorescent Mechanochromism and Thermochromism.
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Reaction of [Au(tht)](ClO) (tht = tetrahydrothiophene), [Cu(CHCN)](ClO), 3,6-di--butyl-1,8-diethynyl-9-carbazole (Hdecz), and bis(2-diphenylphosphinophenyl)ether (POP) in the presence of triethylamine (NEt) gave the cluster complex AuCu(decz)(POP) as yellow crystals. As revealed by X-ray crystallography, the AuCu cluster exhibits scissor-like structure sustained by two decz and two POP ligands and stabilized by Au-Cu and Au-Au interactions. The AuCu cluster shows bright yellow to orange photoluminescence upon irradiation at >300 nm, arising from [π (decz)→5d (Au)] LMCT (ligand-to-metal charge transfer) and [π→π* (decz)] IL (intraligand) triplet states as revealed by theoretical and computational studies.
View Article and Find Full Text PDFCupriphication of gold to sensitize d-d metal-metal bonds and near-unity phosphorescence quantum yields.
Proc Natl Acad Sci U S A
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Department of Chemistry, University of North Texas, Denton, TX 76203;
Outer-shell s/p orbital mixing with d orbitals and symmetry reduction upon cupriphication of cyclic trinuclear trigonal-planar gold(I) complexes are found to sensitize ground-state Cu(I)-Au(I) covalent bonds and near-unity phosphorescence quantum yields. Heterobimetallic AuCu {[Au(μ-C,N-EtIm)Cu(µ-3,5-(CF)Pz)], (4a)}, AuCu {[Au(μ-C,N-BzIm)Cu(µ-3,5-(CF)Pz)], (1) and [Au(μ-C,N-MeIm)Cu(µ-3,5-(CF)Pz)], (3a)}, AuCu {[Au(μ-C,N-MeIm)Cu(µ-3,5-(CF)Pz)], (3b) and [Au(μ-C,N-EtIm)Cu(µ-3,5-(CF)Pz)], (4b)} and stacked Au/Cu {[Au(μ-C,N-BzIm)][Cu(µ-3,5-(CF)Pz)], (2)} form upon reacting Au {[Au(μ-C,N-(N-R)Im)] ((N-R)Im = imidazolate; R = benzyl/methyl/ethyl = BzIm/MeIm/EtIm)} with Cu {[Cu(μ-3,5-(CF)Pz)] (3,5-(CF)Pz = 3,5-bis(trifluoromethyl)pyrazolate)}. The crystal structures of 1 and 3a reveal stair-step infinite chains whereby adjacent dimer-of-trimer units are noncovalently packed via two Au(I)⋯Cu(I) metallophilic interactions, whereas 4a exhibits a hexanuclear cluster structure wherein two monomer-of-trimer units are linked by a genuine d-d polar-covalent bond with ligand-unassisted Cu(I)-Au(I) distances of 2.
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Inorg Chem
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School of Chemistry, Queen's University Belfast, UK.
Changes in the optical properties of an alkynyldigold(I) complex upon reaction with Cu(I) are associated with a complicated structural change to form an unusual Au4Cu2 cluster with metallophilic interactions as well as pi-alkyne coordination.
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