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 Cr1+m
Se2(001)/CuCr2Se4(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.