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Abstract: We have obtained several charge-transfer complexes of CnDTP-TTF (n =5,6). The C5DTP-TTF salts are the κ-type semiconductor with high room-temperature conductivities, whereas β′′-(C6DTP-TTF)2(GaCl4)0.66 shows the metallic behavior down to 40K. In order to improve the conductivity by increasing the bandwidth, we have applied a pressure and synthesized a series of the selenium analogues, CnDTP-STF (n =5,6). In this report, crystal structures and conducting behaviors of CnDTP-TTF salts, and the attempt of increasing the bandwidths are described. [Copyright &y& Elsevier]

Abstract: A new series of RDT-EDO-TTF [R =C5, C6, C7, C8; (cis-l,2-cycloalkylene-l,2-dithio)ethylenedioxytetrathiafulvalene and R =Bz; (benzodithio)ethylenedioxytetrathiafulvalene] donors containing cycloalkylene or benzene, and ethylenedioxy groups as a source of the steric hindrance and the intermolecular hydrogen bonds has been synthesized. The charge transfer (CT) salts, β″-(RDT-EDO-TTF)2(PF6)x (R =C5, C6, C7, C8, and Bz), have the similar β″-type donor arrangement due to the intermolecular hydrogen-bonded network (CH…O) in the two-dimensional (2D) plane. The C6DT-EDO-TTF molecule containing the flexible cyclohexylene group affords the 2:1 salts, which shows the metallic behaviors down to 1.3K with a variety of resistivities at room temperature, 3.0×10−3∼5.0×10−2 ohmcm. On the other hand, the BzDT-EDO-TTF donor with the fixed functional benzo group gives the non-stoichiometry complexes, which exhibit the similar metallic behavior down to 1.3K with the largest RRR=40∼115 among the RDT-EDO-TTF salts. [Copyright &y& Elsevier]