Oxidation-controlled magnetism and Verwey transition in Fe/Fe3O4 lamellae

The structural and magnetic properties of Fe/Fe3O4 nanocomposites, synthesized by combined high energy ball milling and controlled oxidation, have been studied. An X-ray diffraction analysis of the crystal structure of the nanocomposites confirmed the coexistence of Fe and Fe3O4 phases. An increase of the oxygen concentration during oxidation process led to the formation of a higher fraction of the Fe3O4 phase with good crystallinity and stoichiometry. The morphology of the nanocomposites revealed a lamella-like structure with a thickness of about 30 nm. The saturation magnetization decreased when the phase fraction of Fe3O4 increased. The coercivity was enhanced at low temperatures (≤100 K) but decreased at high temperatures, due to thermal fluctuation effects on the anisotropy in the Fe3O4 phase. Interestingly, the lamellae exhibited a sharp Verwey transition near 120 K, which is often suppressed or absent in nanostructured Fe3O4 due to the poorly crystalline, off-stoichiometric characteristic. The temperature dependence of high-field magnetization of the lamellae is analyzed by the modified Bloch law. Our study demonstrates the possibility of tuning the magnetism in iron/iron oxide nanosystems through controlled oxidation.