We have fabricated thin films of a van der Waals (vdW) ferromagnetic metal Fe5GeTe2 and characterized them by measuring the anomalous Hall effect. While the bulk Fe5GeTe2 does not exhibit a perpendicular magnetic anisotropy (PMA) unlike Fe3GeTe2, PMA emerges in the thin film devices. Furthermore, the PMA is enhanced with decreasing the thickness of Fe5GeTe2. In particular, a thin film (5 unit-cell layer) device fabricated with Fe5GeTe2 quenched at 1050 K has two times larger coercive field than that prepared without quenching. Such a PMA should be useful for future vdW spintronic devices.

We have performed magnetoresistance (MR) measurements on van der Waals ferromagnetic devices using quenched- (Q-) and nonquenched- (NQ-) Fe5GeTe2 crystals. A clear butterfly-shaped hysteresis has been observed for thin-film (less than 6 unit-cell layer) Q- and NQ-Fe5GeTe2 devices, but not for thicker film ones. The switching field of the butterfly-shaped MR is consistent with the coercive filed obtained from the Hall measurements. The MR ratio of the butterfly peak reaches about 10% at maximum, which is much larger than that observed with conventional magnetic materials. Such a large MR ratio would be related to magnetic fluctuations due to the complicated magnetic structure in this material.

We investigate near-Fermi-energy (EF) element-specific electronic and spin states of ferromagnetic van der Waals (vdW) metal Fe5GeTe2. The soft x-ray angle-resolved photoemission spectroscopy (SX-ARPES) measurement provides spectroscopic evidence of localized Fe 3d band. We also find prominent hybridization between the localized Fe 3d band and the delocalized Ge/Te p bands. This picture is strongly supported from direct observation of the remarkable spin polarization of the ligand p bands near EF, using x-ray magnetic circular dichroism (XMCD) measurements. The strength of XMCD signal from ligand element Te shows the highest value, as far as we recognize, among literature reporting finite XMCD signal for none-magnetic element in any systems. Combining SX-ARPES and elemental selective XMCD measurements, we collectively point an important role of giant spin polarization of the delocalized ligand Te states for realizing itinerant long-range ferromagnetism in Fe5GeTe2. Our finding provides a fundamental elemental selective view-point for understanding mechanism of itinerant ferromagnetism in low dimensional compounds, which also leads insight for designing exotic magnetic states by interfacial band engineering in heterostructures.