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A first coordination [2.2.2]cryptand(K+)2FeII(TI˙-)(TI2-)2·2C6H4Cl2 (1) complex of iron(ii) containing radical anions and dianions of thioindigo (TI) was obtained. The complex has two high-spin FeII centers bound by two oxygen atoms, and the TI˙- radical anions are coordinated to each FeII. As a result, the 4-spin system consisting of TI˙- (S = 1/2)-FeII (S = 2)-FeII (S = 2)-TI˙- (S = 1/2) coupled spins is formed within a dimer with strong FeII-FeII (J = -51.1 cm-1) and weaker FeII-TI˙- interactions of (J = -35.4 cm-1).We describe the fu
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