Toward 2D Magnets in the (MnBi₂Te₄)(Bi₂Te₃)_n Bulk Crystal

Abstract 2D magnets and their engineered magnetic heterostructures are intriguing materials for both fundamental physics and application prospects. On the basis of the recently discovered intrinsic magnetic topological insulators (MnBi₂Te₄)(Bi₂Te₃)_n, here, a new type of magnet, in which the magnetic layers are separated by a large number of non‐magnetic layers and become magnetically independent, is proposed. This magnet is named as a single‐layer magnet, regarding the vanishing interlayer exchange coupling. Theoretical calculations and magnetization measurements indicate that, the decoupling of the magnetic layers starts to emerge from n = 2 and 3, as revealed by a unique slow‐relaxation behavior below a ferromagnetic‐type transition at T_c = 12–14 K. Magnetization data analysis shows that the proposed new magnetic states have a strong uniaxial anisotropy along the c‐axis, forming an Ising‐type magnetic structure, where T_c is the ordering temperature for each magnetic layer. The characteristic slow relaxation, which exists only along the c‐axis but is absent along the ab plane, can be ascribed to interlayer coherent spin rotation and/or intralayer domain wall movement. The present results will stimulate further theoretical and experimental investigations for the prototypical magnetic structures, and their combination with the topological surface states may lead to exotic physical properties.