Room-temperature ferromagnetism in Ni(II)-chromia based core-shell nanoparticles: experiment and first principles calculations

We have synthesized bimagnetic core-shell nanoparticles containing a first-of-its-kind Ni(II)-chromia nanophase shell and a well-defined, epitaxial core-shell interface. Magnetic measurements reveal a substantial coercivity of the nanoparticles and a significant exchange bias effect between the antiferro-magnetic chromia core and the ferro-magnetic Ni(II)-chromia shell at low temperatures. The ferromagnetism and a weak exchange bias effect are found to persist to room temperature in the core-shell nanoparticles of similar to 57 nm average size. Our first principles Density Functional Theory (DFT) calculations confirm that the novel corundum-structured Ni(II)-chromia phase has an equilibrium cluster-localized ferromagnetic spin configuration. In addition, the DFT-based calculations show that the Ni(II)-chromia phase is a Mott-Hubbard insulator, with a narrowed energy band gap and increased covalent bonding due to strong hybridization between Ni 3d and O 2p levels in the upper portion of the valence band and within the band gap region. The antiferromagnetic, ferromagnetic and magnetoelectric properties of our core-shell nanoparticles make these well suited for patterned recording media and biomedical applications.