Competition between the Direct Exchange Interaction and Superexchange Interaction in Layered Compounds LiCrSe₂, LiCrTe₂, and NaCrTe₂ with a Triangular Lattice

Physical properties of new S = 3/2 triangular-lattice compounds LiCrSe₂, LiCrTe₂, and NaCrTe₂ have been investigated by X-ray diffraction and magnetic measurements. These compounds crystallize in the ordered NiAs-type structure, where alkali metal ions and Cr atoms stack alternately. Despite their isomorphic structures, magnetic properties of these three compounds are different; NaCrTe₂ has an A-type spin structure with ferromagnetic layers, LiCrTe₂ is likely to exhibit a helical spin structure, and LiCrSe₂ shows a first-order-like phase transition from the paramagnetic trigonal phase to the antiferromagnetic monoclinic phase. In these compounds and the other chromium chalcogenides with a triangular lattice, we found a general relationship between the Curie–Weiss temperature and magnetic structures. This relation indicates that the competition between the antiferromagnetic direct d-d exchange interaction and the ferromagnetic superexchange interaction plays an important role in determining the ground state of chromium chalcogenides.