期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 17, 期 1, 页码 130-142出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201001965
关键词
acetylides; cyclometalation; excited states; gold; luminescence
资金
- The University of Hong Kong
- World Gold Council
- URC Strategic Research Theme on Molecular Materials
- University Grants Committee (UGC) Areas of Excellence Scheme [AoE/P-03/08, SEG_HKU07]
- Innovation and Technology Fund (ITF) [ITS/142/08]
A novel class of luminescent dialkynylgold(III) complexes containing various phenylpyridine and phenylisoquinoline-type bidentate ligands has been successfully synthesized and characterized. The structures of some of them have also been determined by X-ray crystallography. Electrochemical studies demonstrate the presence of a ligand-centered reduction originating from the cyclometalating (CN)-N-boolean AND ligand, whereas the first oxidation wave is associated with an alkynyl ligand-centered oxidation. The electronic absorption and photoluminescence properties of the complexes have also been investigated. In dichloromethane solution at room temperature, the low-energy absorption bands are assigned as the metal-perturbed pi-pi* intraligand (IL) transition of the cyclometalating (CN)-N-boolean AND ligand, with mixing of charge-transfer character from the aryl ring to the pyridine or isoquinoline moieties of the cyclometalating (CN)-N-boolean AND ligand. The low-energy emission bands of the complexes in fluid solution at room temperature are ascribed to originate from the metal-perturbed pi-pi* IL transition of the cyclometalatng (CN)-N-boolean AND ligand. For complex 4 that contains an electron-rich amino substituent on the alkynyl ligand, a structureless emission band, instead of one with vibronic structures as in the other complexes, was observed, which was assigned as being derived from an excited state of a [pi(C CC6H4NH2)->pi*((CN)-N-boolean AND)] ligand-to-ligand charge-transfer (LLCT) transition.
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