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Atomically Defined Templates for Epitaxial Growth of Complex Oxide Thin Films
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Layer Resolved Cr Oxidation State Modulation in Epitaxial SrFe0.67Cr0.33O3-δ Thin Films.

Krishna Prasad Koirala1, Mohammad Delower Hossain1, Le Wang1

  • 1Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States.

Nano Letters
|October 31, 2024
PubMed
Summary

Doping SrFe0.67Cr0.33O3-δ thin films with iron and chromium alters their structure and oxidation states. This B-site cation doping in perovskite oxides reduces the optical bandgap, enhancing functionalities.

Keywords:
STEM/EELSSrFeO2.5brownmilleritecation dopingepitaxial thin films

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Oxide Electronics

Background:

  • Perovskite oxides (ABO3) are crucial for various electronic applications.
  • Understanding doping effects on their physicochemical properties is key to functional tuning.
  • SrFexCr1-xO3-δ systems offer a platform to study B-site cation interactions.

Purpose of the Study:

  • Investigate the impact of Fe and Cr competition on the structure of SrFe0.67Cr0.33O3-δ epitaxial thin films.
  • Determine the B-site cation oxidation states and their correlation with structural changes.
  • Elucidate the role of oxygen vacancies in driving charge disproportionation.

Main Methods:

  • Epitaxial thin film growth of SrFe0.67Cr0.33O3-δ.
  • Structural characterization using electron energy loss spectroscopy (EELS).
  • Theoretical simulations (density functional theory) to model electronic structure and bonding.

Main Results:

  • Observed coexistence of perovskite-like and brownmillerite-like structures within the films.
  • Fe remained as Fe3+, while Cr exhibited mixed valencies (Cr3+, Cr4+, and Cr4.5+) depending on the local environment.
  • Cr charge disproportionation was linked to Cr-O bond arrangements and oxygen vacancy interactions.
  • Optical bandgap reduction from ~2.0 eV to ~1.7 eV due to high-valent Cr cations.

Conclusions:

  • B-site cation doping in perovskite oxides significantly influences structural and electronic properties.
  • Cr charge disproportionation is a key mechanism affecting the electronic structure and optical properties.
  • These findings provide insights for designing functional perovskite materials through controlled doping.