Van der Waals Chromium Telluride Thin Films Prepared by Hybrid Pulsed Laser Deposition With Tunable Magnetism

Flexible growth techniques provide a promising pathway toward controlled materials synthesis. We report the epitaxial growth of van der Waals (vdW) Cr (1+δ) Te 2 materials on Al 2 O 3 (0001) substrates using a hybrid Pulsed Laser Deposition (h‐PLD) endorsed by molecular beam source. In a UHV chamber, Cr ablation driven by a pulsed laser is synergistically combined with simultaneous Te molecular evaporation, to grow CrTe 2 (δ = 0) and Cr 2 Te 3 (δ = 1/3) epitaxial thin films. The Cr (1+δ) Te 2 /Al 2 O 3 films show a ferro‐paramagnetic phase transition, with the Curie temperature (T C ) increasing from ∼125 K for CrTe 2 (δ = 0) to ∼325 K for Cr 2 Te 3 (δ = 1/3). Notably, CrTe 2 (δ = 0) thin films display perpendicular magnetic anisotropy, which transitions to in‐plane magnetic anisotropy for Cr 2 Te 3 (δ = 1/3) due to the incorporation of Cr intercalants (δ). The films exhibit robust stability in ambient air, assessed by long‐term magnetization measurements. Negative magnetoresistance with a butterfly magnetoresistance for CrTe 2 , as well as anomalous Hall effects, were observed in both compositions. Above T C , the Cr intercalation in Cr 2 Te 3 alters the dominant charge carrier distribution, demonstrated by a sign change of the Hall coefficient in Cr 2 Te 3 . This work highlights h‐PLD as a promising technique to grow vdW materials and emphasizes the potential of Chromium Tellurides for spintronics applications.