Journal
INORGANIC CHEMISTRY
Volume 44, Issue 12, Pages 4157-4165Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ic048311o
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Several new dinitritochromium(III) complexes of the type trans-[Cr(L)(ONO)(2)]BF4,where L is a derivative of the macrocyclic ligand cyclam having pendant aromatic chromophores attached (L = 5,7-dimethyl-6-(substituted)1,4,8,11-tetraazacyclotetradecane), have been prepared and characterized. Photoexcitation of aqueous solutions containing these complexes at wavelengths corresponding to the pendant chromophore absorption bands led to the generation of NO as detected by an electrochemical sensor. Photophysical data show that the expected fluorescence of the pendant chromophores is largely quenched when the macrocyclic ligand is coordinated to these Cr(III) centers, and this is interpreted in terms of fast energy transfer processes from the ligand-centered pi pi* states to the Cr(III)-centered ligand field states leading to subsequent cleavage of the Cr(III)-coordinated nitrito ligand. Thus, the chromophores tethered to the coordinated cyclam serve as light-gathering antennae for the intramolecular sensitization of the NO-generating photoreactions at the metal center.
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