The diimine compound 1- [(2Ј,3Ј,4Ј,5Ј-tetraphenylbiphenyl-4yl)methyl]-2-(pyridin-2-yl)-1H-benzo[d]imidazole (Ph 6 PyMz) has been designed and synthesized in order to prepare [Cu(Ph 6 PyMz)(DPEphos)]BF 4 {DPEphos = bis[2-(diphenylphosphanyl)phenyl] ether} and [RePh 6 PyMz(CO) 3 Br]. The molecular structures of [Cu(Ph 6 PyMz)(DPEphos)]BF 4 and [RePh 6 PyMz(CO) 3 Br] were determined by single-crystal Xray diffraction and IR spectroscopy, and their properties were systematically studied by thermal-stability analyses, photophysical analyses, and electrochemistry. It was found that [Cu(Ph 6 PyMz)(DPEphos)]BF 4 and [RePh 6 PyMz(CO) 3 Br] mainly give triplet-ligand-to-ligand charge-transfer transition emission in CH 2 Cl 2 solution and pure triplet-metal-to-[a]
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