Tailoring magnetic properties of Cr2Te3 via selective Se substitution

Magnetic two-dimensional (2D) heterostructures have garnered substantial attention due to their advantages in spintronic applications. However, obtaining a perfect interface is still challenging owing to unavoidable dislocations or a mismatch between different 2D magnets. In this work, a highly tunable magnetism has been achieved in Cr2Te3 via selective Se substitution, which is promising for overcoming the above issue. The magnetic ground state of Cr2(SexTe1−x)3 can be adjusted from canted-ferromagnetism (x = 0) to easy-axis collinear-ferromagnetism (x = 0.13), which is accompanied by a large coercivity of about 5800 Oe, and even to isotropic antiferromagnetism (x ≥ 0.25). First-principles calculations reveal that different ground states are mainly attributed to the variation of the interlayer exchange interaction J2. Thus, the Cr2(SexTe1−x)3, with controllable magnetism, is promising for constructing magnetic heterojunctions, where the magnetism on both sides of the interface can be flexibly tailored for diverse demands.