The metamagnetic behavior of the low temperature properties of single crystal Co(pyridine)2Cl2 is discussed. At 1.25 K oriented single crystals exhibit a two‐step metamagnetic transition at applied fields ∼0.8 and 1.6 kG along the b‐axis, a single transition at ∼0.7 kG for applied fields along the a axis, and a single transition at ∼4.2 kG for an applied field along the c axis. Just above the transition fields a moment of 2μB/Co atom is measured for B0 parallel to the a axis or b axis, and 0.4μB/Co atom is measured for the B0 parallel to the c axis. A large field dependent moment is observed at high fields. Many features of this compound closely mirror the behavior of CoCl2⋅2H2O. However, the Co(pyridine)2Cl2 has a much smaller interchain exchange, so that many features can be examined at lower fields. The basic features are consistent with a six‐sublattice model for the ordered antiferromagnetic system. Measurements of magnetic moment versus temperature show that Co(pyridine)2Cl2 does not obey a Curie–Weiss law even at relatively high temperatures.



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