Phase composition and magnetic characteristics of Fe-filled multi-walled carbon nanotubes

The work addresses the correlation between the phase composition and the magnetic characteristics of aligned Fe-filled multi-walled carbon nanotubes (Fe-MWCNTs) grown by pyrolysis of ferrocene on oxidized Si substrates. In a combinatorial approach we exploited the extremely high gradients of the technological parameters temperature and ferrocene flow across the surface of a substrate positioned close to the reactor wall to obtain a large variation in the structural and magnetic properties of the Fe-MWCNTs. In this way, we established several clear correlations between the Fe-filling phase composition and the overall magnetic characteristics of the aligned Fe-MWCNTs. The α-Fe rich samples, which possess a more ordered graphitic sheet structure, a higher degree of preferred crystalline orientation of the metal filling and much larger metal crystallites in comparison with the carbide-rich samples, show a much stronger magnetic anisotropy with easy axis perpendicular to the substrate and unusually high values of the coercive field Hc and the saturation field Hs. The changes in the measured saturation magnetisation Ms and the Hc values correlate well with the variation of the α-Fe content and the filling crystallinity. A special annealing treatment of the samples causes a distinct increase of the α-Fe quantity and an increase of the measured average grain size. The respective magnetic characteristics show a significant increase of the overall magnetic moment and decrease of the coercive field. The correlation between the structural and the magnetic characteristics of the annealed samples matches quite well the respective correlations in the case of as-deposited samples.