Planar Heterojunction of Ultrathin CrTe₃ and CrTe₂ van der Waals Magnet

The fabrication of planar heterojunctions with magnetic van der Waals ultrathin crystals is essential for constructing miniaturized spintronic devices but is yet to be realized. Here, we report the growth of CrTe3 and CrTe2 ultrathin films with molecular beam epitaxy and characterize their morphological and electronic structure through low-temperature scanning tunneling microscopy/spectroscopy. The former is identified as a Mott insulator, and the latter has shown a robust magnetic order previously. Through vacuum annealing, CrTe3 can be transformed into CrTe2, whose relative ratio is controlled via the annealing time. This renders the feasibility of constructing CrTe3–CrTe2 planar heterojunctions, which express atomically sharp interfaces and smooth band bending. We also identified a superstructure conceivably formed via hybrid units of CrTe3 and CrTe2, whose electronic structure exhibits stunning tunability with the length of the superstructure. Our study sets a foundation for the development of magnetic tunneling junctions for building spintronic circuits and engineering electronic states in artificial superlattice structures.