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- ItemEpitaxial stannate pyrochlore thin films: Limitations of cation stoichiometry and electron doping(Melville, NY : AIP Publishing, 2021) Hensling, Felix V. E.; Dahliah, Diana; Dulal, Prabin; Singleton, Patrick; Sun, Jiaxin; Schubert, Jürgen; Paik, Hanjong; Subedi, Indra; Subedi, Biwas; Rignanese, Gian-Marco; Podraza, Nikolas J.; Hautier, Geoffroy; Schlom, Darrell G.We have studied the growth of epitaxial films of stannate pyrochlores with a general formula A2Sn2O7 (A = La and Y) and find that it is possible to incorporate ∼25% excess of the A-site constituent; in contrast, any tin excess is expelled. We unravel the defect chemistry, allowing for the incorporation of excess A-site species and the mechanism behind the tin expulsion. An A-site surplus is manifested by a shift in the film diffraction peaks, and the expulsion of tin is apparent from the surface morphology of the film. In an attempt to increase La2Sn2O7 conductivity through n-type doping, substantial quantities of tin have been substituted by antimony while maintaining good film quality. The sample remained insulating as explained by first-principles computations, showing that both the oxygen vacancy and antimony-on-tin substitutional defects are deep. Similar conclusions are drawn on Y2Sn2O7. An alternative n-type dopant, fluorine on oxygen, is shallow according to computations and more likely to lead to electrical conductivity. The bandgaps of stoichiometric La2Sn2O7 and Y2Sn2O7 films were determined by spectroscopic ellipsometry to be 4.2 eV and 4.48 eV, respectively. © 2021 Author(s).
- ItemAdsorption-controlled growth of La-doped BaSnO3 by molecular-beam epitaxy(Melville, NY : AIP Publ., 2017) Paik, Hanjong; Chen, Zhen; Lochocki, Edward; Seidner H., Ariel; Verma, Amit; Tanen, Nicholas; Park, Jisung; Uchida, Masaki; Shang, ShunLi; Zhou, Bi-Cheng; Brützam, Mario; Uecker, Reinhard; Liu, Zi-Kui; Jena, Debdeep; Shen, Kyle M.; Muller, David A.; Schlom, Darrell G.Epitaxial La-doped BaSnO3 films were grown in an adsorption-controlled regime by molecular-beam epitaxy, where the excess volatile SnOx desorbs from the film surface. A film grown on a (001) DyScO3 substrate exhibited a mobility of 183 cm2 V-1 s-1 at room temperature and 400 cm2 V-1 s-1 at 10 K despite the high concentration (1.2 × 1011 cm-2) of threading dislocations present. In comparison to other reports, we observe a much lower concentration of (BaO)2 Ruddlesden-Popper crystallographic shear faults. This suggests that in addition to threading dislocations, other defects - possibly (BaO)2 crystallographic shear defects or point defects - significantly reduce the electron mobility.