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Strain-induced creation and switching of anion vacancy layers in perovskite oxynitrides.

ABSTRACT: Perovskite oxides can host various anion-vacancy orders, which greatly change their properties, but the order pattern is still difficult to manipulate. Separately, lattice strain between thin film oxides and a substrate induces improved functions and novel states of matter, while little attention has been paid to changes in chemical composition. Here we combine these two aspects to achieve strain-induced creation and switching of anion-vacancy patterns in perovskite films. Epitaxial SrVO₃ films are topochemically converted to anion-deficient oxynitrides by ammonia treatment, where the direction or periodicity of defect planes is altered depending on the substrate employed, unlike the known change in crystal orientation. First-principles calculations verified its biaxial strain effect. Like oxide heterostructures, the oxynitride has a superlattice of insulating and metallic blocks. Given the abundance of perovskite families, this study provides new opportunities to design superlattices by chemically modifying simple perovskite oxides with tunable anion-vacancy patterns through epitaxial lattice strain.

SUBMITTER: Yamamoto T

PROVIDER: S-EPMC7683707 | biostudies-literature | 2020 Nov

REPOSITORIES: biostudies-literature

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Strain-induced creation and switching of anion vacancy layers in perovskite oxynitrides.

Yamamoto Takafumi T Chikamatsu Akira A Kitagawa Shunsaku S Izumo Nana N Yamashita Shunsuke S Takatsu Hiroshi H Ochi Masayuki M Maruyama Takahiro T Namba Morito M Sun Wenhao W Nakashima Takahide T Takeiri Fumitaka F Fujii Kotaro K Yashima Masatomo M Sugisawa Yuki Y Sano Masahito M Hirose Yasushi Y Sekiba Daiichiro D Brown Craig M CM Honda Takashi T Ikeda Kazutaka K Otomo Toshiya T Kuroki Kazuhiko K Ishida Kenji K Mori Takao T Kimoto Koji K Hasegawa Tetsuya T Kageyama Hiroshi H

Nature communications 20201123 1

Perovskite oxides can host various anion-vacancy orders, which greatly change their properties, but the order pattern is still difficult to manipulate. Separately, lattice strain between thin film oxides and a substrate induces improved functions and novel states of matter, while little attention has been paid to changes in chemical composition. Here we combine these two aspects to achieve strain-induced creation and switching of anion-vacancy patterns in perovskite films. Epitaxial SrVO<sub>3</ ...[more]

PMID: 33230157

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Project description:Layered perovskites have been extensively investigated in many research fields, such as electronics, catalysis, optics, energy, and magnetics, because of the fascinating chemical properties that are generated by the specific structural features of perovskite frameworks. Furthermore, the interlayers of these structures can be chemically modified through ion exchange to form nanosheets. To further expand the modification of layered perovskites, we have demonstrated an advance in the new structural concept of layered perovskite "charge-neutral perovskite layers" by manipulating the perovskite layer itself. A charge-neutral perovskite layer in [CeIVTa2O7] was synthesized through a soft chemical oxidative reaction based on anionic [CeIIITa2O7]- layers. The Ce oxidation state for the charge-neutral [CeIVTa2O7] layers was found to be tetravalent by X-ray absorption fine structure (XAFS) analysis. The atomic arrangements were determined through scattering transmission electron microscopy and extended XAFS (EXAFS) analysis. The framework structure was simulated through density functional theory (DFT) calculations, the results of which were in good agreement with those of the EXAFS spectra quantitative analysis. The anionic [CeIIITa2O7]- layers exhibited optical absorption in the near infrared (NIR) region at approximately 1000 nm, whereas the level of NIR absorption decreased in the [CeIVTa2O7] charge-neutral layer due to the disappearance of the Ce 4f electrons. In addition, the chemical reactivity of the charge-neutral [CeIVTa2O7] layers was investigated by chemical reduction with ascorbic acid, resulting in the reduction of the [CeIVTa2O7] layers to form anionic [CeIIITa2O7]- layers. Furthermore, the anionic [CeIIITa2O7]- layers exhibited redox activity which the Ce in the perovskite unit can be electrochemically oxidized and reduced. The synthesis of the "charge-neutral" perovskite layer indicated that diverse features were generated by systematically tuning the electronic structure through the redox control of Ce; such diverse features have not been found in conventional layered perovskites. This study could demonstrate the potential for developing innovative, unique functional materials with perovskite structures.

Dataset Information

Strain-induced creation and switching of anion vacancy layers in perovskite oxynitrides.

Publications

Strain-induced creation and switching of anion vacancy layers in perovskite oxynitrides.

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