Itinerant ferromagnetism in van der Waals Fe5−xGeTe2 crystals above room temperature

Two-dimensional (2D) van der Waals (vdW) magnets have recently attracted increasing attention, as they provide a novel system for exploring 2D magnetism. However, intrinsic ferromagnetism in 2D systems has almost exclusively been observed at low temperatures, limiting their technological relevance. ${\mathrm{Fe}}_{\mathrm{N}}{\mathrm{Ge}\mathrm{Te}}_{2}$ ($N=3$, 4, and 5) systems are currently becoming the most attractive 2D vdW materials due to their relatively high Curie temperatures and large saturation magnetization. However, the nature of their complex yet intriguing magnetic behaviors is still unclear, in part due to the multiple inequivalent iron sites and iron vacancies. Here, we show evolution of magnetic ordering transitions in ${\mathrm{Fe}}_{5\ensuremath{-}x}{\mathrm{Ge}\mathrm{Te}}_{2}$ with high Curie temperature and a strong saturation magnetization using photoemission electron microscopy and transport measurements. At 275 K, the ferromagnet transitions to a ferrimagnet, and below 110 K transitions to a state with glassy clusters. These are evidenced from temperature-dependent magnetic stripe domain evolution and anisotropic magnetoresistance measurements. Our findings show a clear magnetic ground state of ${\mathrm{Fe}}_{5\ensuremath{-}x}{\mathrm{Ge}\mathrm{Te}}_{2}$ at room temperature which signals that ${\mathrm{Fe}}_{5\ensuremath{-}x}{\mathrm{Ge}\mathrm{Te}}_{2}$ system is a very promising candidate for spintronic devices and provides a material design pathway to further increase the Curie temperature and saturation moments in vdW ferromagnets.