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Two-dimensional (2D) magnetic transition metal compounds with atomicthickness exhibit intriguing physics in fundamental research and greatpotential for device applications. Understanding the correlations between theirmacrosopic magnetic properties and the dimensionality of microscopic magneticexchange interactions are valuable for the designing and applications of 2Dmagnetic crystals. Here, using spin-polarized scanning tunneling microscopy,magnetization and magneto-transport measurements, we identify thezigzag-antiferromagnetism in monolayer CrTe2, incipient ferromagnetism inbilayer CrTe2, and robust ferromagnetism in bilayer Cr3Te4 films. Our densityfunctional theory calculations unravel that the magnetic ordering in ultrathinCrTe2 is sensitive to the lattice parameters, while robust ferromagnetism withlarge perpendicular magnetic anisotropy in Cr3Te4 is stabilized through itsanisotropic 3D magnetic exchange interactions.

Tuning the Magnetism in Ultrathin CrxTey Films by Lattice Dimensionality