Intralayer antiferromagnetism in two-dimensional van der Waals magnet Fe$_3$GeTe$_2$

Abstract: For the van der Waals magnet Fe$_3$GeTe$_2$, although a ferromagnetic ground state has been reported, there are also reports of complex magnetic behavior suggesting coexistence of ferromagnetism and antiferromagnetism due to the intricate interaction between Fe$^{+3}$ and Fe$^{+2}$ ions in this system. The exact nature of the interactions and the origin of antiferromagnetism are still under debate. Here, we report the observation of signature of ferromagnetic and antiferromagnetic couplings between different Fe-ions in the anomalous Hall effect measured for devices of mechanically exfoliated Fe$_3$GeTe$_2$ nano-flakes of thicknesses ranging from\,$\sim$\,15-20 layers. The temperature-dependent anomalous Hall effect data reveal two sharp step-like switchings at low temperature ($T\lesssim150\,$K). Our detailed analyses suggest the step-like sharp switchings in anomalous Hall resistance are due to the magnetization reversal behavior of different Fe-ions in individual layers of Fe$_3$GeTe$_2$. The experimental results can be explained by considering an intra-layer antiferromagnetic coupling between Fe$^{+3}$ and Fe$^{+3}$ ions, whereas intra-layer ferromagnetic coupling between Fe$^{+3}$ and Fe$^{+2}$ in the system. Our experimental results and the analyses are supported by the first-principles calculations for energetics and intralayer as well as interlayer exchange coupling constants.