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    Suitability of binary oxides for molecular-beam epitaxy source materials: A comprehensive thermodynamic analysis
    (Melville, NY : AIP Publ., 2020) Adkison, Kate M.; Shang, Shun-Li; Bocklund, Brandon J.; Klimm, Detlef; Schlom, Darrell G.; Liu, Zi-Kui
    We have conducted a comprehensive thermodynamic analysis of the volatility of 128 binary oxides to evaluate their suitability as source materials for oxide molecular-beam epitaxy (MBE). 16 solid or liquid oxides are identified that evaporate nearly congruently from stable oxide sources to gas species: As2O3, B2O3, BaO, MoO3, OsO4, P2O5, PbO, PuO2, Rb2O, Re2O7, Sb2O3, SeO2, SnO, ThO2, Tl2O, and WO3. An additional 24 oxides could provide molecular beams with dominant gas species of CeO, Cs2O, DyO, ErO, Ga2O, GdO, GeO, HfO, HoO, In2O, LaO, LuO, NdO, PmO, PrO, PuO, ScO, SiO, SmO, TbO, Te2O2, U2O6, VO2, and YO2. The present findings are in close accord with available experimental results in the literature. For example, As2O3, B2O3, BaO, MoO3, PbO, Sb2O3, and WO3 are the only oxides in the ideal category that have been used in MBE. The remaining oxides deemed ideal for MBE awaiting experimental verification. We also consider two-phase mixtures as a route to achieve the desired congruent evaporation characteristic of an ideal MBE source. These include (Ga2O3 + Ga) to produce a molecular beam of Ga2O(g), (GeO2 + Ge) to produce GeO(g), (SiO2 + Si) to produce SiO(g), (SnO2 + Sn) to produce SnO(g), etc.; these suboxide sources enable suboxide MBE. Our analysis provides the vapor pressures of the gas species over the condensed phases of 128 binary oxides, which may be either solid or liquid depending on the melting temperature. © 2020 Author(s).
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    Self-stabilization of the equilibrium state in ferroelectric thin films
    (Amsterdam : Elsevier, 2022) Gaal, Peter; Schmidt, Daniel; Khosla, Mallika; Richter, Carsten; Boesecke, Peter; Novikov, Dmitri; Schmidbauer, Martin; Schwarzkopf, Jutta
    (K,Na)NbO3 is a lead-free and sustainable ferroelectric material with electromechanical parameters comparable to Pb(Zr,Ti)O3 (PZT) and other lead-based solid solutions. It is therefore a promising candidate for caloric cooling and energy harvesting applications. Specifically, the structural transition from the low-temperature Mc- to the high-temperature c-phase displays a rich hierarchical order of domains and superdomains, that forms at specific strain conditions. The relevant length scales are few tens of nanometers for the domain and few micrometers for the superdomain size, respectively. Phase-field calculations show that this hierarchical order adds to the total free energy of the solid. Thus, domains and their formation has a strong impact on the functional properties relevant for electrocaloric cooling or energy harvesting applications. However, monitoring the formation of domains and superdomains is difficult and requires both, high spatial and high temporal resolution of the experiment. Synchrotron-based time-resolved X-ray diffraction methods in combination with scanning imaging X-ray microscopy is applied to resolve the local dynamics of the domain morphology with sub-micrometer spatial and nanosecond temporal resolution. In this regime, the material displays a novel self-stabilization mechanism of the domain morphology, which may be a general property of first-order phase transitions.