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The experimental charge distribution in sulfur‐containing molecules. Structure determination and electron density study of NaSCN at reduced temperatures

The crystal structure of NaSCN (sodium thiocyanate) has been determined by X-ray diffraction studies at 150 and 81 K and a neutron diffraction study at about 94 K. The space group of the structure is Pmcn, the molecules being arranged in the mirror planes. The SCN group is approximately linear with CS and CN bond lengths of 1. 647 (1) and 1. 178 (I) /k respectively. Deformation density maps calculated from the 150 K and 81 K X-ray data are very similar. The deformation density around the C and N atoms suggests sphybridization, while the S lone-pair electrons are found in a diffuse ring around the S atom perpendicular to the C S bond, indicating an almost unhybridized S atom. A charge-population analysis assigns a net charge of +0.27 (6) e to the Na atom.