Abstract
We report magnetic and structural studies on the two-dimensional antiferromagnets (MCl)LaNb2O7 (M = Mn, Cr, Co), prepared by topochemical reactions of a layered perovskite RbLaNb2O7. Electron diffraction of these oxyhalides revealed a superstructure with a \(\sqrt{2}a \times \sqrt{2}a \) cell for M = Mn and Co, and a 2a × 2a cell for M = Cr, indicating that the MCl networks are distorted from an ideal square lattice. Neutron diffraction experiments showed that M = Mn and Co exhibit a \((\pi 0 )\) antiferromagnetic order as observed for the S = 1/2 counterparts. (CoCl)LaNb2O7 with a strong spin anisotropy shows an antiferro to weak-ferromagnetic transition at low field, followed by novel two-step metamagnetic transitions likely associated with a 1/2 plateau for 27–54 T. Possible spin structures under magnetic field are discussed in terms of an Ising-type model. By contrast, (CrCl)LaNb2O7 exhibits a \((\pi \pi )\) order, which is the first observation among related oxyhalides, and a spin-flop tr...
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