From ferromagnetic semiconductor to antiferromagnetic metal in epitaxial CrxTey monolayers

Abstract Chromium ditelluride, CrTe₂, is an attractive candidate van der Waals material for hosting 2D magnetism. However, how the room-temperature ferromagnetism of the bulk evolves as the sample is thinned to the single-layer limit has proved controversial. This, in part, reflects its metastable nature, vs. a series of more stable self-intercalation compounds with higher relative Cr:Te stoichiometry. Here, exploiting a recently developed method for enhancing nucleation in molecular-beam epitaxy growth of transition-metal chalcogenides, we demonstrate the selective stabilisation of high-coverage CrTe₂ and Cr_2+ε Te₃ epitaxial monolayers. Combining X-ray magnetic circular dichroism, scanning tunnelling microscopy, and temperature-dependent angle-resolved photoemission, we demonstrate that both compounds order magnetically with a similar T _C. We find, however, that monolayer CrTe₂ forms as an antiferromagnetic metal, while monolayer Cr_2+ε Te₃ hosts an intrinsic ferromagnetic semiconducting state. This work thus demonstrates that control over the self-intercalation of metastable Cr-based chalcogenides provides a powerful route for tuning both their metallicity and magnetic structure, establishing the Cr_xTe_y system as a flexible materials class for future 2D spintronics.