Disentangling the unusual magnetic anisotropy of the near-room-temperature ferromagnet Fe$_{4}$GeTe$_{2}$

TL;DR

This study uses electron spin resonance to analyze the complex magnetic anisotropy of Fe$_{4}$GeTe$_{2}$, revealing temperature-dependent behaviors that link magnetic and electronic properties, with implications for 2D magneto-electronic applications.

Contribution

It provides the first quantitative ESR insights into the unusual magnetic anisotropy and its temperature evolution in Fe$_{4}$GeTe$_{2}$, highlighting the coupling between magnetic and electronic degrees of freedom.

Findings

Magnetic anisotropy is dominated by demagnetization at high temperatures.

Intrinsic magnetic anisotropy grows below 150 K, affecting isotropy at 110 K.

Complex intrinsic anisotropy appears below 50 K, matching transport measurement signatures.

Abstract

In the quest for two-dimensional 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 $T_\mathrm{SR} \sim 110$ 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-D 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 $T_{\rm shape} \sim 150$ K renders the sample seemingly isotropic at $T_\mathrm{SR}$. Below one further temperature $T_{\rm d} \sim 50$ 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.