X-ray structures for tetramethyl-p-urazine 1 and its dithia derivative 3 show these compounds to exist in significantly twisted boat structures with nearly planar nitrogens. The X-ray structure of the fused bicyloco-[2.2. 2loctyl derivative cation radical 4*+ is consistent with a delocalized structure having equivalent NN bonds and planar nitrogens. ESR and ENDOR data are consistent with delocalized cation radicals in solution. Cyclic ...