'Colossal magnetoresistance' in perovskite manganites such as La0.7Ca0.3MnO3 (LCMO), is caused by the interplay of ferro-paramagnetic, metal-insulator and structural phase transitions. Moreover, different electronic phases can coexist on a very fine scale resulting in percolative electron transport. Here we report on (LCMO)1-x:(MgO)x (0 < x < or = 0.8) epitaxial nano-composite films in which the structure and magnetotransport properties of the manganite nanoclusters can be tuned by the tensile stress originating from the MgO second phase. With increasing x, the lattice of LCMO was found to expand, yielding a bulk tensile strain. The largest colossal magnetoresistance of 10(5)% was observed at the percolation threshold in the conductivity at xc 0.3, which is coupled to a structural phase transition from orthorhombic (0 < x < or 0.1) to rhombohedral R3c structure (0.33 < or = x < or = 0.8). An increase of the Curie temperature for the Rc phase was observed. These results may provide a general method for controlling the magnetotransport properties of manganite-based composite films by appropriate choice of the second phase.

Epitaxial La(3/4)Ca(1/4)MnO3/MgO(100) (LCMO) thin film shows an unusual rhombohedral (R-3c) structure with a new perovskite superstructure at room temperature due to the CE-type ordering of La and Ca with modulation vector q=1/4[011]. A-site ordered film was found to be electronically homogeneous down to the 1 nm scale as revealed by scanning tunnelling microscopy/spectroscopy. In contrast, orthorhombic and A-site disordered LCMO demonstrate a mesoscopic phase separation far below the Curie temperature (TC). Unique La/Ca ordering compensates the cation mismatch stress within one supercell, a(S) approximately 1.55 nm, and enhances the electronic homogeneity. The phase separation does not seem to be a unique mechanism for the colossal magnetoresistance (CMR) as very large CMR approximately 500% was also observed in A-site ordered films.

Microstructural and magnetic properties of (La0.7Sr0.3MnO3)0.7:(Mn3O4)0.3 nanocomposite thin films