Tunable magnetic properties in van der Waals crystals (Fe$_{1-x}$Co$_x$)$_5$GeTe$_2$

Abstract: We report the doping effects of cobalt on van der Waals (vdW) magnet Fe$5$GeTe$_2$. A series of (Fe${1-x}$Co$x$)$_5$GeTe$_2$ (0$\leq$x$\leq$0.44) single crystals have been successfully grown, their structural, magnetic and transport properties are investigated. For x=0.20, The Curie temperature $T_C$ increases from 276~K to 337~K. Moreover, the magnetic easy-axis is reoriented to the $ab$-plane from the $c$-axis in undoped Fe$_5$GeTe$_2$ with largely enhanced magnetic anisotropy. These magnetic properties would make (Fe${0.8}$Co${0.2}$)$_5$GeTe$_2$ more effective in stabilizing magnetic order in the two-dimensional limit. A complex magnetic phase diagram is identified on the higher doping side. The x=0.44 crystal first orders ferromagnetically at $T_C$=363~K then undergoes an antiferromagnetic transition at $T_N$=335~K. Furthermore magnetic-field-induced spin-flop transitions are observed for the AFM ground state. Our work reveals (Fe${1-x}$Co$_x$)$_5$GeTe$_2$ as promising candidates for developing new spin-related applications and proposes a method to engineer the magnetic properties of vdW magnet.