The results of molecular orbital calculations are presented in an attempt to answer four questions concerning the electronic structure of N4S4 and its derived ions. The important conclusions are: (1) A geometrical structure involving coplanar nitrogen atoms is to be preferred over one involving coplanar sulfur atoms. (2) Appreciable bonding is to be expected between sulfur atoms located on the same side of the plane defined by the four nitrogen atoms. No bonding is to be expected between nitrogen atoms. (3) Negative ions of N4S4 having one to four units of charge ought to exist and exhibit x-electron-delocalized electronic structures.
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