Four new neutral copper-azido polymers [Cu4(N3)8(Me-hmpz)2]n (1), [Cu4(N3)8(men)2]n (2), [Cu5(N3)10(N,N-dmen)2]n (3) and [Cu5(N3)10(N,N′-dmen)5]n (4) [Me-hmpz = 1-methylhomopiperazine; men = N-methylethylenediamine; N,N-dmen = N,N-dimethylethylenediamine and N,N′-dmen = N,N′-dimethylethylenediamine] have been synthesized by using various molar equivalents of the chelating diamine ligands with Cu(NO3)2·3H2O and an excess of NaN3. Single-crystal X-ray structures show that the basic asymmetric units of 1 and 2 are very similar, but the overall 1D structures were found to be quite different. Complex 3 with a different composition was found to be 2D in nature, while the 1D complex 4 with 1 : 1 metal to diamine ratio presented several new structural features. Cryomagnetic susceptibility measurements over a wide range of temperature were corroborated with density functional theory calculations (B3LYP functional) performed on the complexes 1–3 to provide a qualitative theoretical interpretation of their overall magnetic behavior.
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