Atomic Scale Characterization of Complex Oxide Thin Films

Materials with the ABO3 perovskite structure possess a wide variety of properties including superconductivity, ferroelectric, and magnetic properties. The understanding of the structure-property relationship for several different systems of perovskite oxide thin films and superlattices were developed on the atomic scale.;Multifunctional superlattices composed of ferromagnetic (FM) La 0.7Sr0.3MnO3 (LSMO) and antiferromagnetic (AFM) La0.7Sr0.3FeO3 (LSFO) have potential applications for next generation data storage and logic devices. Defect formation, driven by strain relaxation in the LSMO/LSFO superlattices can modify not only the structure and surface sharpness, but also the functional properties of the superlattice. Stacking faults were found as one efficient way of strain relaxation while maintaining robust antiferromagnetic properties for a thin [3LSMO][6LSFO] superlattice (repeating motif composed of 3 unit-cell LSMO sublayer and 6 unit-cell LSFO sublayer). On the other hand, for a fully strained [3LSMO][6LSFO], large inter-diffusion across the interface between the LSMO and LSFO layers was detected in EELS line scans, resulting in deteriorated AFM properties. When a [6LSMO][6LSFO] superlattice with one micron thickness, a high density of nanoflowers and cracks/pinholes were observed to result from strain relaxation. The formation of these nanoflowers and cracks/pinholes was suppressed by increasing the growth rate and thereby reducing the growth time and overall thermal treatment of the sample.;A series of superlattices composed of non-magnetic La0.5Sr 0.5TiO3 (LSTO) and ferromagnetic LSMO were grown on single crystal oxide substrates with different amounts of misfit strain. No significant electronic structure changes along the interfaces was observed in this series of superlattices as revealed by atomic resolution EELS. In comparison, charge transfer effect was reported for the LSMO/STO superlattices and was shown to cause an ultrathin magnetic dead layer along the interfaces. Thus, compared with the LSMO/STO superlattice, composition tuning of the sublayers was proven to be efficient in controlling the interfacial charge transfer effects in a superlattice. In addition, tetragonal distortion was found to reduce the ferromagnetic ordering, decrease the Tc, increase the resistivity, and even lead to metal-insulator transitions of the superlattices. The strain relaxation defects such as dislocations and low angle grain boundaries serve as important pinning sites for magnetic domains, leading to enhanced coercive field strength.;In order to determine the properties of an intermixed interface layer, we have performed a detailed study of the solid solution between LSMO and LSFO, i.e. La0.7Sr0.3Mn0.5Fe0.5O 3 (LSMFO). A large target-substrate distance during the PLD growth led to cation segregation in the LSMFO film. Cation segregation could cause the formation of diverse local magnetic ordering and B site valence states due to the different local stoichiometry and coordination environment. For the cation segregated LSFMO films, robust ferromagnetic and antiferromagnetic coupling was observed at 150K and room temperature. Decreasing the target-substrate distance resulted to a homogeneous cation distribution in the film, without any ferromagnetic ordering as expected. This result suggests the important role of target-substrate distance and the kinetic energy of the plume species on the crystalline quality and functional properties of perovskite oxide thin films.;LaxSr1-xTiO3 possesses a wide range of functional properties which make it an attractive candidate material for applications such as the conductive buffer for high temperature superconductor growth, transparent conductors, and anodes in solid oxide fuel cells. La 0.5Sr0.5TiO3 thin films were grown using PLD and the resistivity was found to be highly dependent on the O2 background pressure used in the deposition. However, a thin film which was deposited as a single phase film was transformed into a semi-ordered superlattice with TiO2 rich stacking faults and distorted lattices upon exposure to high oxygen pressure (∼200torr) during the cooling procedure after deposition. This phase change stabilized Ti4+ ions and dramatically increased the resistivity of the film. (Abstract shortened by UMI.).