期刊
INORGANIC CHEMISTRY
卷 48, 期 5, 页码 2094-2102出版社
AMER CHEMICAL SOC
DOI: 10.1021/ic801987t
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资金
- Academy of Finland
- Russian Foundation [07-03-00908-a]
The reactions between the diphosphino-alkynyl gold complexes (XC6H4C2Au)PR2-C6H4-PR2(AuC2C6H4X) with Cu+ lead to the formation of a family of heterometallic clusters of the general formula [{Au3Cu2(C2C6H4X)(6)}-Au-3(PR2C6H4PR2)(3)][PF6](2) (X = NO2, H, OMe, NMe2; R = C6H5, NC4H4). These complexes adopt the same structural pattern and consist of a heterometallic alkynyl cluster [Au3Cu2(C2C6H4X)(6)](-) wrapped by the cationic [Au-3(PR2C6H4PR2)(3)](3+) belt. The novel compounds were characterized by NMR spectroscopy and ESI-MS measurements. A systematic study of their luminescence properties revealed efficient room-temperature phosphorescence in solution with remarkably weak quenching by molecular oxygen. The photophysical experiments demonstrate that the increase in the electron donor ability of the alkynyl ligands and the electron-withdrawing character of the diphosphines results in the bathochromic shift of emission maxima (in the 576-686 nm range) and a decrease in the luminescence quantum yield. The electronic structure calculations showed that variations of X or R substituents have very little effect on the structural parameters but display a significant influence on the electronic properties of the clusters and characteristics of luminescence. The metal-centered triplet emission within the heterometallic alkynyl cluster is suggested to play a key role in the observed phosphorescence.
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