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Out-of-phase boundaries (OPBs) are translation boundary defects characterized by a misregistry of a fraction of a unit cell dimension in neighboring regions of a crystal. Although rarely observed in the bulk, they are common in epitaxial films of complex crystals due to the physical constraint of the underlying substrate and a low degree of structural rearrangement during growth. OPBs can strongly affect properties, but no extensive studies of them are available. The morphology, structure, and nucleation mechanisms of OPBs in epitaxial films of layered complex oxides are presented with a review of published studies and new work. Morphological trends in two families of layered oxide phases are described. The atomic structure at OPBs is presented. OPBs may be introduced into a film during growth via the primary mechanisms that occur at film nucleation (steric, nucleation layer, a-bmisfit, and inclined-cmisfit) or after growth via the secondary nucleation mechanism (crystallographic shear in response to loss of a volatile component). Mechanism descriptions are accompanied by experimental examples. Alternative methods to the direct imaging of OPBs are also presented.
Portions of the same epitaxial (103)-oriented SrBi2Nb2O9 film grown on (111) SrTiO3 for which we recently reported the highest remanent polarization (Pr) ever achieved in SrBi2Nb2O9 (or SrBi2Ta2O9) films, i.e., Pr = 15.7 μC/cm2, have been characterized microstructurally by plan-view and cross-sectional transmission electron microscopy (TEM) along three orthogonal viewing directions. SrBi2Nb2O9 grows with its c axis tilted 57° from the substrate surface normal in a three-fold twin structure about the substrate , with the growth twins' c axes nominally aligned with the three 〈100〉 SrTiO3 directions. (103) SrBi2Nb2O9 films with and without an underlying epitaxial SrRuO3 bottom electrode have been studied. Dark-field TEM imaging over a 12 μm2 area shows no evidence of second phases (crystalline or amorphous). A high density of out-of-phase boundaries exists in the films.
(001)-oriented epitaxial SrBi2Nb2O9 thin films have been grown by pulsed laser deposition on (001) SrTiO3 and (001) LaAlO3—Sr2AlTaO6 substrates at optimized growth conditions. 4-circle x-ray diffraction, Rutherford backscattering spectrometry, and transmission electron microscopy reveal highly oriented epitaxial films. Atomic force microscopy indicates spiral growth for films grown on SrTiO3 and layer-by-layer growth for films grown on LaAlO3—Sr2AlTaO6.
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