magnetic nanoparticles are of immense current interest because of their possible use in biomedical and technological applications. Here we demonstrate that the large magnetic anisotropy of FePt nanoparticles can be significantly modified by surface design. We employ X-ray absorption spectroscopy offering an element-specific approach to magnetocrystalline anisotropy and the orbital magnetism. Experimental results on oxide-free FePt nanoparticles embedded in Al are compared with large-scale density functional theory calculations of the geometric-and spin-resolved electronic structure, which only recently have become possible on world-leading supercomputer architectures. The combination of both approaches yields a more detailed understanding that may open new ways for a microscopic design of magnetic nanoparticles and allows us to present three rules to achieve desired magnetic properties. In addition, concrete suggestions of capping materials for FePt nanoparticles are given for tailoring both magnetocrystalline anisotropy and magnetic moments.

Correlating the electronic structure and magnetic response with the morphology and crystal structure of the same single ferromagnetic nanoparticle has been up to now an unresolved challenge. Here, we present measurements of the element-specific electronic structure and magnetic response as a function of magnetic field amplitude and orientation for chemically synthesized single Fe nanocubes with 18 nm edge length. Magnetic states and interactions of monomers, dimers, and trimers are analyzed by X-ray photoemission electron microscopy for different particle arrangements. The element-specific electronic structure can be probed and correlated with the changes of magnetic properties. This approach opens new possibilities for a deeper understanding of the collective response of magnetic nanohybrids in multifunctional materials and in nanomagnetic colloidal suspensions used in biomedical and engineering technologies.

The reduced magnetic moments of oxide-free FePt nanoparticles are discussed in terms of lattice expansion and local deviation from the averaged composition. By analyses of the extended x-ray absorption fine structure of FePt nanoparticles and bulk material measured both at the Fe K and Pt L(3) absorption edge, the composition within the single nanoparticles is found to be inhomogeneous, i.e. Pt is in a Pt-rich environment and, consequently, Fe is in an Fe-rich environment. The standard Fourier transformation-based analysis is complemented by a wavelet transformation method clearly visualizing the difference in the local composition. The dependence of the magnetic properties, i.e. the element-specific magnetic moments on the composition in chemically disordered Fe(x)Pt(1-x) alloys, is studied by fully relativistic SPR-KKR band structure calculations supported by experimental results determined from the x-ray magnetic circular dichroism of 50 nm thick films and bulk material.

Nearly perfect single crystalline Fe core-shell nanocubes with (100) facets and 13.6 nm edge length were prepared by wet-chemical methods. While the core is metallic, the shell is composed of either Fe3O4 or γ-Fe2O3. The cubes were deposited onto GaAs substrates with monolayer coverage as proved by scanning electron microscopy. Oxygen and hydrogen plasmas were used to remove the ligand system and the oxide shell. Both types of samples were investigated by ferromagnetic resonance. While the g-factor (g=2.09) and crystalline anisotropy (K4=4.8×104 J/m3) of the pure iron cubes show up with bulk values, the saturation magnetization is reduced to (M(5K)=(1.2±0.12)×106 A/m) 70% of bulk value and the effective damping parameter (α=0.03) is increased by one order of magnitude with respect to bulk Fe.

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