Itinerant ferromagnetism mediated by giant spin polarization of the metallic ligand band in the van der Waals magnet \nFe5GeTe2

Abstract

We investigate near-Fermi-energy (${E}_{F}$) element-specific electronic and spin states of ferromagnetic van der Waals (vdW) metal ${\\mathrm{Fe}}_{5}\\mathrm{Ge}{\\mathrm{Te}}_{2}$. 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 ${E}_{F}$, 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 nonmagnetic element in any systems. Combining SX-ARPES and elemental selective XMCD measurements, we collectively point to an important role of giant spin polarization of the delocalized ligand Te states for realizing itinerant long-range ferromagnetism in ${\\mathrm{Fe}}_{5}\\mathrm{Ge}{\\mathrm{Te}}_{2}$. Our finding provides a fundamental elemental selective viewpoint for understanding mechanism of itinerant ferromagnetism in low-dimensional compounds, which also leads to insight for designing exotic magnetic states by interfacial band engineering in heterostructures.