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Register a new userAtomic structure of initial nucleation layer in hexagonal perovskite BaRuO$_3$ thin films
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Hexagonal perovskites are an attractive group of materials due to their various polymorph phases and rich structure-property relationships. BaRuO3 (BRO) is a prototypical hexagonal perovskite, in which the electromagnetic properties are significantly modified depending on its atomic structure. Whereas thin-film epitaxy would vastly expand the application of hexagonal perovskites by epitaxially stabilizing various metastable polymorphs, the atomic structure of epitaxial hexagonal perovskites, especially at the initial growth stage, has rarely been investigated. In this study, we show that an intriguing nucleation behavior takes place during the initial stabilization of a hexagonal perovskite 9R BaRuO3 (BRO) thin film on a (111) SrTiO3 (STO) substrate. We use high-resolution high-angle annular dark field scanning transmission electron microscopy in combination with geometrical phase analysis to understand the local strain relaxation behavior. We find that nano-scale strained layers, composed of different RuO6 octahedral stacking, are initially formed at the interface, followed by a relaxed single crystal9R BRO thin film. Within the interface layer, hexagonal BROs are nucleated on the STO (111) substrate by both corner- and face-sharing. More interestingly, we find that the boundaries between the differently-stacked nucleation layers, i.e. heterostructural boundaries facilitates strain relaxation, in addition to the formation of conventional misfit dislocations evolving from homostructural boundaries. Our observations reveal an important underlying mechanism to understand the thin-film epitaxy and strain accommodation in hexagonal perovskites.
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We report on the observation of metallic behavior in thin films of oxygen-deficient SrTiO$_3$ - down to 9 unit cells - when coherently strained on (001) SrTiO$_3$ or DyScO$_3$-buffered (001) SrTiO$_3$ substrates. These films have carrier concentrations of up to 2$times10^{22}$ cm$^{-3}$ and mobilities of up to 19,000 cm$^2$/V-s at 2 K. There exists a non-conducting layer in our SrTiO$_{3-delta}$ films that is larger in films with lower carrier concentrations. This non-conducting layer can be attributed to a surface depletion layer due to a Fermi level pinning potential. The depletion width, transport, and structural properties are not greatly affected by the insertion of a DyScO$_3$ buffer between the SrTiO$_3$ film and SrTiO$_3$ substrate.
Advances in synthesis techniques and materials understanding have given rise to oxide heterostructures with intriguing physical phenomena that cannot be found in their constituents. In these structures, precise control of interface quality, including oxygen stoichiometry, is critical for unambiguous tailoring of the interfacial properties, with deposition of the first monolayer being the most important step in shaping a well-defined functional interface. Here, we studied interface formation and strain evolution during the initial growth of LaAlO3 on SrTiO3 by pulsed laser deposition, in search of a means for controlling the atomic-sharpness of the interfaces. Our experimental results show that growth of LaAlO3 at a high oxygen pressure dramatically enhances interface abruptness. As a consequence, the critical thickness for strain relaxation was increased, facilitating coherent epitaxy of perovskite oxides. This provides a clear understanding of the role of oxygen pressure during the interface formation, and enables the synthesis of oxide heterostructures with chemically-sharper interfaces.
Although enhanced conductivity at ferroelectric domain boundaries has been found in BiFeO$_3$ films, Pb(Zr,Ti)O$_3$ films, and hexagonal rare-earth manganite single crystals, the mechanism of the domain wall conductivity is still under debate. Using conductive atomic force microscopy, we observe enhanced conductance at the electrically-neutral domain walls in semiconducting hexagonal ferroelectric TbMnO$_3$ thin films where the structure and polarization direction are strongly constrained along the c-axis. This result indicates that domain wall conductivity in ferroelectric rare-earth manganites is not limited to charged domain walls. We show that the observed conductivity in the TbMnO$_3$ films is governed by a single conduction mechanism, namely, the back-to-back Schottky diodes model tuned by the segregation of defects.
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