| Abstract
| - The reaction of LnI3·xMeCN (Ln = Gd, Dy) and TCNE (tetracyanoethylene) in acetonitrile forms Ln2[C4(CN)8]3·xMeCN. These paramagnetic light-colored solids contain the S = 0 octacyanobutandiide dianion, [C4(CN)8]2-,which upon desolvation of these products forms dark green Ln(TCNE)3. In these compounds the central C−C σbond in [C4(CN)8]2- is broken, re-forming S = 1/2 [TCNE]•-. as evidenced by the color change and the infraredspectra. Ln(TCNE)3 exhibit coupling between Ln3+ and [TCNE]•- and magnetically order as ferrimagnets at 8.5(Dy) and 3.5 (Gd) K.
- Reaction of LnI3·xMeCN (Ln = Gd, Dy) and TCNE forms Ln2[C4(CN)8]3·xMeCN, which upon desolvation forms Ln(TCNE)3. Ln2[C4(CN)8]3·xMeCN is paramagnetic, as it possesses the S = 0 octacyanobutanediide dianion, while Ln(TCNE)3, which possesses S = 1/2 [TCNE]•- that couples to Ln3+, magnetically orders as a ferrimagnet at 8.5 (Dy) and 3.5 (Gd) K.
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