Pairs of stacks of organic donors D in the salt [(DT‐TTF)2][Au(mnt)2] (DT‐TTF = dithiophene‐tetrathiafulvalene, mnt = maleonitriledithiolate) form a classical ladder structure due to three close S …︁ S interactions (see picture). Below 225 K the double stack of donor molecules forms a spin ladder with two legs, which arises through localization of unpaired electrons in the (DT‐TTF)2 dimers.

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The nickel complex nBu 4 N[Ni(α-tpdt) 2 ] (2) (α-tpdt = 2,3-thiophenedithiolate) has been prepared and characterized. A salt of this monoanionic paramagnetic complex, [Fe(Cp* ) 2 ][Ni(α-tpdt) 2 ] (3), was obtained with decamethylferrocene, crystallizing in the monoclinic space group P2 1 /a with a = 15.443(3), b = 10.237(1), c = 20.360(2) Å , β = 107.54(1)°, V = 3069.1(7) Å 3 , Z = 4. Its structure consists of alternating cationic and anionic layers, with short interlayer contacts defining alternating cation−anion chains. Magnetic characterization of 3 at low applied magnetic fields revealed an antiferro-

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