Anomalous magnetic properties of quasi two-dimensional van der Waals ferromagnet Fe4GeTe2

Abstract

We have studied the magnetic properties of quasi two-dimensional itinerant ferromagnet Fe${}_4$GeTe${}_2$ as functions of temperature and magnetic field ($B$) with field parallel to the $ab$-plane ($B\Vert ab$) and $c$-axis ($B\Vert c$) of the crystal. This van der Waals compound undergoes a continuous paramagnetic to ferromagnetic phase transition below $T_C$ = 270.0 K and a pronounced spin reorientation transition at around $T_{SR}$ $\sim$ 115 K where the easy axis of magnetization changes its direction from in-plane to out-of-plane. The temperature evolution of magnetization in the FM state is highly anomalous and extremely sensitive to the direction and strength of applied magnetic field. Magnetic entropy change ($\Delta S_M$) has been estimated in the vicinity of $T_C$ and $T_{SR}$. $\Delta S_M$($T$) is found to be almost isotropic around $T_C$ while it shows very unusual behavior and is sensitive to the direction of applied field at low temperature close to $T_{SR}$. For $B\Vert c$, $\Delta S_M$ is negative and decreases continuously with field and -$\Delta S_M$($T$) shows a broad maximum around $T_{SR}$ similar to that observe at $T_C$. On the other hand, $\Delta S_M$ is positive in the vicinity of $T_{SR}$ below 1.4 T and -$\Delta S_M$($T$) exhibits a peak at $T_{SR}$ which becomes very sharp at high field for $B\Vert ab$. These results suggest complex nature of the magnetic ground state of Fe${}_4$GeTe${}_2$, which is possibly due to the presence of multiple inequivalent Fe sites, their ordering and complexity of spin configuration.