The crystal structures of uncharged tetrahedral dithiocyanato zinc com
plexes with N-methylated ethyienediamines have been determined with a
view to a study of intermolecular hydrogen-bonding interactions in the
se compounds. It is found that the H(N) hydrogen atoms are exhaustivel
y engaged in N-H(N)... S bonds. The majority of these bonds are branch
ed (bifurcated or trifurcated), and the hydrogen-bond systems they for
m all contain one of the two characteristic primitive core motifs: eit
her a discrete centrosymmetric [... S ... H ...](2) dimer or an infini
te [... S ... H ...](infinity) helix about a 2(1) or pseudo-2(1) axis.
The hydrogen bonding is analyzed in detail, with particular attention
to the existence of correlations between the N-H(N)-S angles and the
H(N)... S distances as well as between the corresponding N-H(N)-S/H(N)
... S pairs in the bifurcated N-H(N)... 2S bonds.