Abstract

An efficient synthesis of one new (10) and three previously reported (9, 11, and 12) π-electron donors, which have one sulfur atom in each of the outer five-membered rings attached to the TTF system, is presented. The radical cations derived from (9-11) have been studied by ESR spec- troscopy and the spin density distribution of these radical cations, as well as those of other related radical cations, have been determined by MO calculations and correlated with the ESR spectral data. The single- crystal X-ray structures of π-donors (9) and (12) are reported. The most remarkable fact of these structures is the transverse intermolecular contacts between interstacked molecules. The external sulfur atoms of (9) play a central role in its transverse structural pattern. Complexes of donors (9) and (10) with tetracyano-p-quinodimethane (TCNQ) and te- trafluorotetracyano-p-quinodimethane (TCNQF 4 ) have been obtained and characterized

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