Epitaxial PbTiO3 thin films were produced from a mixed Pb–Ti double-alkoxide precursor by spin-coating onto single crystal (001) SrTiO3 substrates. Heat treatment at 800 °C produces a dense and continuous, epitaxial lead titanate film through an intermediate Pb-Ti fluorite structure. A microstructural instability occurred when very thin single crystal films were fabricated; this instability caused the films to become discontinuous. Scanning electron microscopy and atomic force microscopy observations show that single crystal films with a thickness less than ∼80 nm developed holes that expose the substrate; thinner films broke up into isolated, single crystal islands. The walls of the holes were found to be (111) perovskite planes. A free energy function, which considered the anisotropic surface energies of different planes, was developed to describe the microstructural changes in the film and to understand the instability phenomenon. The function predicted that pre-existing holes greater than a critical size are necessary to initiate hole growth, and it predicted the observed morphological changes in the current system. Morphological stability diagrams that explain the stability fields for different film configurations, i.e., either completely covered, with holes, or single crystal islands, can be calculated for any film/substrate system.
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