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- ItemGrowth of PdCoO2 films with controlled termination by molecular-beam epitaxy and determination of their electronic structure by angle-resolved photoemission spectroscopy(Melville, NY : AIP Publ., 2022) Song, Qi; Sun, Jiaxin; Parzyck, Christopher T.; Miao, Ludi; Xu, Qing; Hensling, Felix V. E.; Barone, Matthew R.; Hu, Cheng; Kim, Jinkwon; Faeth, Brendan D.; Paik, Hanjong; King, Phil D. C.; Shen, Kyle M.; Schlom, Darrell G.Utilizing the powerful combination of molecular-beam epitaxy (MBE) and angle-resolved photoemission spectroscopy (ARPES), we produce and study the effect of different terminating layers on the electronic structure of the metallic delafossite PdCoO2. Attempts to introduce unpaired electrons and synthesize new antiferromagnetic metals akin to the isostructural compound PdCrO2 have been made by replacing cobalt with iron in PdCoO2 films grown by MBE. Using ARPES, we observe similar bulk bands in these PdCoO2 films with Pd-, CoO2-, and FeO2-termination. Nevertheless, Pd- and CoO2-terminated films show a reduced intensity of surface states. Additionally, we are able to epitaxially stabilize PdFexCo1-xO2 films that show an anomaly in the derivative of the electrical resistance with respect to temperature at 20 K, but do not display pronounced magnetic order.
- 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).
- ItemSynthesis of metastable Ruddlesden–Popper titanates, (ATiO3)nAO, with n ≥ 20 by molecular-beam epitaxy(Melville, NY : AIP Publ., 2022) Barone, Matthew R.; Jeong, Myoungho; Parker, Nicholas; Sun, Jiaxin; Tenne, Dmitri A.; Lee, Kiyoung; Schlom, Darrell G.We outline a method to synthesize (ATiO3)nAO Ruddlesden–Popper phases with high-n, where the A-site is a mixture of barium and strontium, by molecular-beam epitaxy. The precision and consistency of the method described is demonstrated by the growth of an unprecedented (SrTiO3)50SrO epitaxial film. We proceed to investigate barium incorporation into the Ruddlesden–Popper structure, which is limited to a few percent in bulk, and we find that the amount of barium that can be incorporated depends on both the substrate temperature and the strain state of the film. At the optimal growth temperature, we demonstrate that as much as 33% barium can homogeneously populate the A-site when films are grown on SrTiO3 (001) substrates, whereas up to 60% barium can be accommodated in films grown on TbScO3 (110) substrates, which we attribute to the difference in strain. This detailed synthetic study of high n, metastable Ruddlesden–Popper phases is pertinent to a variety of fields from quantum materials to tunable dielectrics