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The yellow compound of stoichiometry (4-chloropyridinium)3Fe2Cl9 belongs to the space group P21/n with four formula units in the unit cell. Structural analysis shows that the iron is present as the FeX4− ion. Magnetic measurements on single crystals show that the material orders as a canted antiferromagnet at 2.725 K. Replacement of the 4-chloro cation by the 4-bromo analog yields an isomorphous material and shifts the transition temperature to 2.34 K. The phase diagrams of both salts have also been determined. For [(4-chloropyridinium)FeCl4]2⋅4-chloropyridinium chloride, the bicritical point is at 2.40 K and 7 kOe, and HSF(0)=5.5 kOe. With Hc(0)=56 kOe, α=HA/HE=1.9×10−2. In the case of [(4-bromopyridinium)FeCl4]2⋅4-bromopyridinium chloride, HSF(0)=3 kOe, Hc(0)=42 kOe, α=1.0×10−2, and the bicritical point is at 2.24 K and 4.2 kOe. Crystallographic investigations at 25 K are reported on the isomorphous (4-chloropyridinium)3Fe2Br9 and on (4-bromopyridinium)3Fe2Cl1.3Br7.7. Magnetic measurements on single crystals show that (4-bromopyridinium)3Fe2Cl1.3Br7.7 orders as a canted antiferromagnet at 5.67 K, while (4-chloropyridinium)3Fe2Br9 orders similarly at 7.96 K. These compounds behave approximately as S=5/2, three-dimensional Heisenberg antiferromagnets.
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