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Abstract

Cr_(1+δ)Te₂ are pseudo-layered compounds consisting of CrTe₂ transition metal dichalcogenide (TMD) layers with additional (δ) self-intercalated Cr atoms. The recent search for ferromagnetic 2D materials revived the interest into chromium tellurides. Here, Cr_(1+δ)Te₂ nanolayers are epitaxially grown on MoS₂ (0001), forming prototypical van der Waals heterostructures. Under optimized growth conditions, ultrathin films of only two TMD layers with a single intercalated Cr-layer are achieved, forming a 2D sheet with van der Waals surfaces. Detailed compositional and structural characterization by scanning tunneling microscopy, grazing incidence x-ray diffraction, and high-resolution Rutherford backscattering indicate the layer-by-layer growth and that the δ can be tuned by post-growth annealing in a range between ∼0.5 and 1. X-ray magnetic circular dichroism and magnetometry measurements demonstrate that all self-intercalated Cr_(1+δ)Te₂ nanolayers exhibit strong ferromagnetism with magnetic moments larger than 3_μB per Cr-atom. The magnetic properties are maintained in the ultrathin limit of a material with a single intercalation layer. Interestingly, the magnetic anisotropy can be tuned from close to isotropic (δ = 1) to a desirable perpendicular anisotropy for low δ values. Thus, the bottom-up growth of these 2D Cr_(1+δ)Te₂ sheets is a promising approach for designing magnetic van der Waals heterostructures.