Direct observation of elemental fluctuation and oxygen octahedral distortion-dependent charge distribution in high entropy oxides

Lei Su, Huaixun Huyan, Abhishek Sarkar, Wenpei Gao, Xingxu Yan, Christopher Addiego, Robert Kruk, Horst Hahn () and Xiaoqing Pan ()
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Lei Su: University of California
Huaixun Huyan: University of California
Abhishek Sarkar: Technical University Darmstadt
Wenpei Gao: University of California
Xingxu Yan: University of California
Christopher Addiego: University of California
Robert Kruk: Karlsruhe Institute of Technology
Horst Hahn: Technical University Darmstadt
Xiaoqing Pan: University of California

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract The enhanced compositional flexibility to incorporate multiple-principal cations in high entropy oxides (HEOs) offers the opportunity to expand boundaries for accessible compositions and unconventional properties in oxides. Attractive functionalities have been reported in some bulk HEOs, which are attributed to the long-range compositional homogeneity, lattice distortion, and local chemical bonding characteristics in materials. However, the intricate details of local composition fluctuation, metal-oxygen bond distortion and covalency are difficult to visualize experimentally, especially on the atomic scale. Here, we study the atomic structure-chemical bonding-property correlations in a series of perovskite-HEOs utilizing the recently developed four-dimensional scanning transmission electron microscopy techniques which enables to determine the structure, chemical bonding, electric field, and charge density on the atomic scale. The existence of compositional fluctuations along with significant composition-dependent distortion of metal-oxygen bonds is observed. Consequently, distinct variations of metal-oxygen bonding covalency are shown by the real-space charge-density distribution maps with sub-ångström resolution. The observed atomic features not only provide a realistic picture of the local physico-chemistry of chemically complex HEOs but can also be directly correlated to their distinctive magneto-electronic properties.

Date: 2022
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DOI: 10.1038/s41467-022-30018-y

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