Disentangling the Unusual Magnetic Anisotropy of the Near‐Room‐Temperature Ferromagnet Fe 4 GeTe 2

In the quest for 2D conducting materials with high ferromagnetic ordering temperature the new family of the layered Fe n GeTe 2 compounds, especially the near‐room‐temperature ferromagnet Fe 4 GeTe 2 , receives a significant attention. Fe 4 GeTe 2 features a peculiar spin reorientation transition at T SR ≈ 110 K suggesting a non‐trivial temperature evolution of the magnetic anisotropy (MA)—one of the main contributors to the stabilization of the magnetic order in the low‐dimensional systems. An electron spin resonance (ESR) spectroscopic study reported here provides quantitative insights into the unusual magnetic anisotropy of Fe 4 GeTe 2 . At high temperatures the total MA is mostly given by the demagnetization effect with a small contribution of the counteracting intrinsic magnetic anisotropy of an easy‐axis type, whose growth below a characteristic temperature T shape ≈ 150 K renders the sample seemingly isotropic at T SR . Below one further temperature T d ≈ 50 K the intrinsic MA becomes even more complex. Importantly, all the characteristic temperatures found in the ESR experiment match those observed in transport measurements, suggesting an inherent coupling between magnetic and electronic degrees of freedom in Fe 4 GeTe 2 . This finding together with the observed signatures of the intrinsic two‐dimensionality should facilitate optimization routes for the use of Fe 4 GeTe 2 in the magneto‐electronic devices, potentially even in the monolayer limit.