55Mn nuclear magnetic resonance experiments are reported on a series of fully strained epitaxial La(2/3)Ca(1/3)MnO3 thin films on SrTiO3. We have found evidence of multiple phase segregation into ferromagnetic metallic and nonmetallic regions as well as regions that are nonferromagnetic and insulating. These insulating regions are mainly located close to interfaces and may have a significant impact on the performance of spin-tunnel devices. As a result of phase segregation, the ferromagnetic coupling within the metallic regions is depressed. This accounts for the reduction of the Curie temperature and conductivity in nanometric thin films.

We have studied the thickness dependence of the magnetotransport properties of La 2/3 Ca 1/3 MnO 3 thin films epitaxially grown on SrTiO 3 , LaAlO 3 , and NdGaO 3 single-crystalline substrates. When thickness decreases, a global disruption of the magnetoelectronic properties occurs, namely the resistivity and the low-temperature magnetoresistance increase while the metal-to-insulator transition temperature (T P ) is lowered. We state that the electronic properties of these films, especially close to the film/substrate interface, differ from those of the bulk material. This is confirmed by nuclear-magnetic-resonance measurements which provide evidence that these films have an inhomogeneous magnetoelectronic nanostructure with distinguishable regions containing localized charges. These regions are scattered within the films, with a higher density close to interfaces in the case of La 2/3 Ca 1/3 MnO 3 films on SrTiO 3 but more homogeneously distributed for films grown on NdGaO 3 . Since our manganite films have a virtually unrelaxed crystal structure, the thickness dependence of T P can neither be related to the strain states nor to dimensional effects. Alternatively, we show that the coexistence of different electronic phases leads to a modification of the carrier density in the metallic regions and, presumably, to an enhancement of the disorder in the Mn-O bond length and Mn-O-Mn angles. We will argue that the conjunction of both factors promotes a decrease of the double exchange transfer integral and, consequently, accounts for the reduction of the Curie temperature for the thinnest films. The possible mechanisms responsible for this phase separation are discussed in terms of the microstructure of the interfaces between the manganite and the insulating perovskite.

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