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Abstract: The synthesis and the redox behaviour of electroactive donor molecules incorporating an azino spacer group between a benzoselenazole core and another heterocyclic moiety, either a benzoselenazole one or a thiazole one, are reported. Neutral complexes were obtained with TCNQ and, for the first time with dithiadiazafulvalene or diselenadiazafulvalene derivatives, cation radical salts by electrocrystallization. Crystal structures data of these complexes are presented and their geometries compared with those deduced from theoretical calculations. [Copyright &y& Elsevier]

Abstract: The synthesis of the protected TTF tetrathiolate 2,3,6,7-tetrakis(2-cyanoethylthio)tetrathiafulvalene (TCE-TTF), as well as those of five new radical cation salts [TCE-TTF](X), X− =PF6 −, CF3SO3 −, BF4 −, obtained by electrocrystallization technique is presented. Five crystal structures of these materials based on their fully oxidized donor molecules are described. The flexibility of the cyanoethylene arm yields two conformations cis and trans to the molecule. Then compounds with PF6 − and BF4 − anions crystallized as two different phases. All these materials are insulators, and the magnetic studies of one phase of [TCE-TTF](PF6) revealed an antiferromagnetic behavior. [Copyright &y& Elsevier]