Ferromagnetism of sputtered Fe3GeTe2 ultrathin films in the absence of two-dimensional crystalline order

The discovery of ferromagnetism in two-dimensional (2D) monolayers has stimulated growing research interest in both spintronics and material science. However, these 2D ferromagnetic layers are mainly prepared through an incompatible approach for large-scale fabrication and integration, and moreover, a fundamental question whether the observed ferromagnetism actually correlates with the 2D crystalline order has not been explored. Here, we choose a typical 2D ferromagnetic material, Fe3GeTe2, to address these two issues by investigating its ferromagnetism in an amorphous state. We have fabricated nanometer-thick amorphous Fe3GeTe2 films approaching the monolayer thickness limit of crystallized Fe3GeTe2 (0.8 nm) through magnetron sputtering. Compared to crystallized Fe3GeTe2, we found that the basic ferromagnetic attributes, such as the Curie temperature that directly reflects magnetic exchange interactions and local anisotropic energy, do not change significantly in the amorphous states. This is attributed to that the short-range atomic order, as confirmed by valence state analysis, is almost the same for both phases. The persistence of ferromagnetism in the ultrathin amorphous counterpart has also been confirmed through magnetoresistance measurements, where two unconventional switching dips arising from electrical transport within domain walls are clearly observed in the amorphous Fe3GeTe2 single layer. These results indicate that the long-range ferromagnetic order of crystallized Fe3GeTe2 may not correlate to the 2D crystalline order and the corresponding ferromagnetic attributes can be utilized in an amorphous state which suits large-scale fabrication in a semiconductor technology-compatible manner for spintronics applications.