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Layer Resolved Cr Oxidation State Modulation in Epitaxial SrFe0.67Cr0.33O3−δ Thin Films

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    Layer Resolved Cr Oxidation State Modulation in Epitaxial SrFe0.67Cr0.33O3−δ Thin Films
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    Nano Letters

    Cite this: Nano Lett. 2024, 24, 45, 14244–14251
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    https://doi.org/10.1021/acs.nanolett.4c03660
    Published October 31, 2024
    Copyright © 2024 American Chemical Society
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    Abstract

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    Understanding how doping influences physicochemical properties of ABO3 perovskite oxides is critical for tailoring their functionalities. In this study, SrFe0.67Cr0.33O3−δ epitaxial thin films were used to examine the effects of Fe and Cr competition on structure and B-site cation oxidation states. The films exhibit a perovskite-like structure near the film/substrate interface, while a brownmillerite-like structure with horizontal oxygen vacancy channels predominates near the surface. Electron energy loss spectroscopy shows Fe remains Fe3+, while Cr varies from ∼Cr3+ (tetrahedral layers) to ∼Cr4+ (octahedral layers) within brownmillerite phases and becomes ∼Cr4.5+ in perovskite-like phases. Theoretical simulations indicate that Cr–O bond arrangements and the way oxygen vacancies interact with Cr and Fe drive Cr charge disproportionation. High-valent Cr cations introduce additional densities of states near the Fermi level, reducing the optical bandgap from ∼2.0 eV (SrFeO2.5) to ∼1.7 eV (SrFe0.67Cr0.33O3−δ). These findings offer insights into B-site cation doping in the perovskite oxide framework.

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.nanolett.4c03660.

    • Methods, RHEED intensity oscillations and images, XRR and RSM, cross-sectional STEM image of the SFCO film on LSAT viewed along the [100] LSAT direction and EDS maps, layer-resolved O K-edge and Fe L-edge spectra through STEM/EELS, and L-edge XAS results (PDF)

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    Nano Letters

    Cite this: Nano Lett. 2024, 24, 45, 14244–14251
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.nanolett.4c03660
    Published October 31, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

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