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Improved Structural Properties in Homogeneously Doped Sm0.4Ce0.6O2−δ Epitaxial Thin Films: High Doping Effect on the Electronic Bands

Cite this: ACS Appl. Mater. Interfaces 2020, 12, 42, 47556–47563
Publication Date (Web):September 28, 2020
https://doi.org/10.1021/acsami.0c13495
Copyright © 2020 American Chemical Society
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Abstract

The study of ionic materials on nanometer scale is of great relevance for efficient miniaturized devices for energy applications. The epitaxial growth of thin films can be a valid route to tune the properties of the materials and thus obtain new degrees of freedom in materials design. High crystal quality SmxCe1–xO2−δ films are here reported at a high doping level up to x = 0.4, thanks to the good lattice matching with the (110) oriented NdGaO3 substrate. X-ray diffraction and transmission electron microscopy demonstrate the ordered structural quality and absence of Sm segregation at the macroscopic and atomic level, respectively. Therefore, in epitaxial thin films, the homogeneous doping can be obtained even with the high dopant content not always approachable in bulk form, getting even an improvement of the structural properties. In situ spectroscopic measurements by X-ray photoemission and X-ray absorption show the O 2p band shift toward the Fermi level, which can favor the oxygen exchange and vacancy formation on the surface when the Sm doping is increased to x = 0.4. X-ray absorption spectroscopy also confirms the absence of ordered oxygen vacancy clusters and further reveals that the 5d eg and t2g states are well separated by the crystal field in the undistorted local structure even in the case of a high doping level up to x = 0.4.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.0c13495.

  • Further X-ray diffraction, X-ray photoemission spectroscopy analysis, further details on the X-ray absorption at the O K-edge, and main chemical reactions involved in SmxCe1–xO2−δ film (PDF)

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  2. S K Chaluvadi, D Mondal, C Bigi, D Knez, P Rajak, R Ciancio, J Fujii, G Panaccione, I Vobornik, G Rossi, P Orgiani. Pulsed laser deposition of oxide and metallic thin films by means of Nd:YAG laser source operating at its 1st harmonics: recent approaches and advances. Journal of Physics: Materials 2021, 4 (3) , 032001. https://doi.org/10.1088/2515-7639/abe661