Substantially Enhanced Spin Polarization in Epitaxial CrTe2 Quantum Films

Abstract 2D van der Waals (vdW) magnets, which extend to the monolayer (ML) limit, are rapidly gaining prominence in logic applications for low‐power electronics. To improve the performance of spintronic devices, such as vdW magnetic tunnel junctions, a large effective spin polarization of valence electrons is highly desired. Despite its considerable significance, direct probe of spin polarization in these 2D magnets has not been extensively explored. Here, using 2D vdW ferromagnet of CrTe 2 as a prototype, the spin degrees of freedom in the thin films are directly probed using Mott polarimetry. The electronic band of 50 ML CrTe 2 thin film, spanning the Brillouin zone, exhibits pronounced spin‐splitting with polarization peaking at 7.9% along the out‐of‐plane direction. Surprisingly, atomic‐layer‐dependent spin‐resolved measurements show a significantly enhanced spin polarization in a 3 ML CrTe 2 film, achieving 23.4% polarization even in the absence of an external magnetic field. The demonstrated correlation between spin polarization and film thickness highlights the pivotal influence of perpendicular magnetic anisotropy, interlayer interactions, and itinerant behavior on these properties, as corroborated by theoretical analysis. This groundbreaking experimental verification of intrinsic effective spin polarization in CrTe 2 ultrathin films marks a significant advance in establishing 2D ferromagnetic atomic layers as a promising platform for innovative vdW‐based spintronic devices.