Effects of the introduction of a chromium oxide monolayer at the C₆₀/Fe(001) interface

The introduction of a two-dimensional oxide layer at the interface between an organic semiconductor and a ferromagnetic metal (spinterface) can help in tailoring the formation of spin-polarized hybridized interface states. Here, we consider the case of a $Cr4O5$ monolayer at the $C60/Fe(001)$ interface, which is already known to feature the occurrence of spin-polarized states in the fullerene molecules. In this work, we employ scanning tunneling microscopy/spectroscopy and photoemission spectroscopy to show that the $C60/Cr4O5/Fe(001)$ spinterface is characterized by the formation of a well-ordered fullerene monolayer and of strongly hybridized interface states. These experimental results are discussed in terms of state-of-the-art ab initio calculations of the structural, electronic, and magnetic properties at the interface.