Origin of the giant magnetic moment in epitaxial Fe3O4 thin films

We study the enhanced magnetic moment observed in epitaxial magnetite (Fe3O4) ultrathin films (t < 15 nm) grown on MgO (001) substrates by means of pulsed laser deposition. The Fe3O4 (001) thin films exhibit high crystallinity, low roughness, and sharp interfaces with the substrate, and the existence of the Verwey transition at thicknesses down to 4 nm. The evolution of the Verwey transition temperature with film thickness shows a dependence with the antiphase boundaries density. Superconducting quantum interference device (SQUID) and vibrating sample magnetometry measurements in ultrathin films show a magnetic moment much higher than the bulk magnetite value. In order to study the origin of this anomalous magnetic moment, polarized neutron reflectivity (PNR), and x-ray magnetic circular dichroism (XMCD) experiments have been performed, indicating a decrease in the magnetization with decreasing sample thickness. X-ray photoemission spectroscopy measurements show no metallic Fe clusters present in the magnetite thin films. Through inductively coupled plasma mass spectroscopy and SQUID magnetometry measurements performed in commercial MgO (001) substrates, the presence of Fe impurities embedded within the substrates has been observed. Once the substrate contribution has been corrected, a decrease in the magnetic moment of magnetite thin films with decreasing thickness is found, in good agreement with the PNR and XMCD measurements. Our experiments suggest that the origin of the enhanced magnetic moment is not intrinsic to magnetite but due to the presence of Fe impurities in the MgO substrates.