Revealing Enhanced Optical Nonlinearity and Robust Ferromagnetism in Atomically Sharp Stacking Binary–Ternary Magnetic Heterostructures

Two-dimensional (2D) materials provide a versatile platform for the integration of diverse crystals, enabling the formation of heterostructures with intriguing functionalities. Coherently growing 2D heterostructures are highly desirable for property manipulation due to their strong interfacial interaction. In this work, we propose a general synthesis approach and provide insight into well-designed 2D binary–ternary magnetic heterostructures. Atomically sharp interfaces were achieved in typical lateral and vertical Cr 1+ m Se 2 (001)/CuCr 2 Se 4 (111) heterostructures owing to their similar lattice arrangement, with the observation of a significant enhancement of optical second-harmonic generation. Further magnetism measurements revealed a Curie temperature up to 360 K and thickness- and temperature-dependent magnetism in this heterostructure. Additionally, we synthesized three analogous 2D magnetic heterostructures in Fe–Cr–S, Co–Cr–S, and Cu–Cr–S systems, demonstrating the ubiquitous nature of the coherent heteroepitaxy. Our work involves the development of an innovative platform for investigating the underlying physics and potential applications of 2D binary–ternary heterostructures as well as the fabrication of associated functional devices.