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Abstract  Two dinuclear complexes with novel coordination type, [Cu2(DPDIDT)2](PF6)2 (1) and [Ag2(DPDIDT)2](BF4)2 (2), plus a dinuclear complex of the usual coordination type, {Re(Cl)(CO)3}2(DPDIDT) (3) as a comparative complex were prepared from bis-(4-(2-pyridylmethyleneiminophenyl))disulfide (DPDIDT) and the relevant metal sources. Complexes (1) and (2) exist in solution as dimer structures of the square-pole type according to the interpretation of the ESI mass and 1H NMR spectra. The density functional theory calculations for the monomer and dimer models of the Cu(I) complex cations, [Cun(DPDIDT)n]n+ (n = 1, 2), demonstrated that the dimer form is structurally more stable than the monomer form. The UV–Vis absorption spectra of complexes (1) and (3) both exhibit a typical MLCT absorption band in the 400–700 nm region. The Re(I) complex (3) was revealed to possess a facial configuration with respect to the three carbonyl ligands by 1H NMR and IR data. [ABSTRACT FROM AUTHOR]