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Jahn–Teller-driven phase segregation in MnxCo3−xO4 spinel thin films

Blanchet, Miles D. ; Matthews, Bethany E. ; Spurgeon, Steven R. ; Heald, Steve M. ; Isaacs-Smith, Tamara ; Comes, Ryan B.

Journal of vacuum science & technology. A, Vacuum, surfaces, and films, 2023-09, Vol.41 (5) [Periódico revisado por pares]

United States: American Vacuum Society / AIP

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  • Título:
    Jahn–Teller-driven phase segregation in MnxCo3−xO4 spinel thin films
  • Autor: Blanchet, Miles D. ; Matthews, Bethany E. ; Spurgeon, Steven R. ; Heald, Steve M. ; Isaacs-Smith, Tamara ; Comes, Ryan B.
  • Assuntos: CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS ; epitaxy ; Jahn-Teller distortion ; stoichiometry ; thin films ; transmission electron microscopy ; x-ray absorption spectroscopy ; x-ray diffraction ; x-ray photoelectron spectroscopy
  • É parte de: Journal of vacuum science & technology. A, Vacuum, surfaces, and films, 2023-09, Vol.41 (5)
  • Notas: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
    PNNL-SA-179218
    National Science Foundation (NSF)
    USDOE Laboratory Directed Research and Development (LDRD) Program
    AC05-76RL01830; AC02-06CH11357; DMR-1809847
    USDOE Office of Science (SC), Biological and Environmental Research (BER)
  • Descrição: Transition metal spinel oxides comprised of earth-abundant Mn and Co have long been explored for their use in catalytic reactions and energy storage. However, understanding functional properties can be challenging due to differences in sample preparation and the ultimate structural properties of the materials. Epitaxial thin film synthesis provides a novel means of producing precisely controlled materials to explore the variations reported in the literature. In this work, MnxCo3−xO4 samples from x = 0 to x = 1.28 were synthesized through molecular beam epitaxy and characterized to develop a material properties map as a function of stoichiometry. Films were characterized via in situ x-ray photoelectron spectroscopy, x-ray diffraction, scanning transmission electron microscopy, and polarized K-edge x-ray absorption spectroscopy. Mn cations within this range were found to be octahedrally coordinated, in line with an inverse spinel structure. Samples largely show mixed Mn3+ and Mn4+ character with evidence of phase segregation tendencies with the increasing Mn content and increasing Mn3+ formal charge. Phase segregation may occur due to structural incompatibility between cubic and tetragonal crystal structures associated with Mn4+ and Jahn–Teller active Mn3+ octahedra, respectively. Our results help in explaining the reported differences across samples in these promising materials for renewable energy technologies.
  • Editor: United States: American Vacuum Society / AIP
  • Idioma: Inglês
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