Stability of the In-Plane Room Temperature van der Waals Ferromagnet Chromium Ditelluride and Its Conversion to Chromium-Interleaved CrTe₂ Compounds

Van der Waals magnetic materials are building blocks for novel kinds of spintronic devices and playgrounds for exploring collective magnetic phenomena down to the two-dimensional limit. Chromium–tellurium compounds are relevant in this perspective. In particular, the 1T phase of CrTe2 has been argued to have a Curie temperature above 300 K, a rare and desirable property in the class of lamellar materials, making it a candidate for practical applications. However, recent literature reveals a strong variability in the reported properties, including magnetic ones. Using electron microscopy, diffraction, and spectroscopy techniques, together with local and macroscopic magnetometry approaches, our work sheds new light on the structural, chemical, and magnetic properties of bulk 1T-CrTe2 exfoliated in the form of flakes having a thickness ranging from few to several tens of nanometers. We unambiguously establish that 1T-CrTe2 flakes are ferromagnetic above room temperature, have an in-plane easy axis of magnetization, and low coercivity, and we confirm that their Raman spectroscopy signatures are two modes: E2g (103.5 cm–1) and A1g (136.5 cm–1). We also prove that thermal annealing causes a phase transformation to monoclinic Cr5Te8 and, to a lesser extent, to trigonal Cr5Te8. In sharp contrast with 1T-CrTe2, none of these compounds have a Curie temperature above room temperature, and they both have perpendicular magnetic anisotropy. Our findings reconcile the apparently conflicting reports in the literature and open opportunities for phase-engineered magnetic properties