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Anomalous Lattice Evolution-Mediated Electrical Properties in Transparent KNN-Based Lead-Free Ferroelectric Films.

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The epitaxial (K0.49Na0.49Li0.02)(Ta0.2Nb0.8)O3 with 2 wt % MnO2 addition (KNNLT-M) film on the transparent La0.03Ba0.97SnO3-coated LaAlO3 (001) substrate is chosen to investigate how the lattice evolution, as well as the… Click to show full abstract

The epitaxial (K0.49Na0.49Li0.02)(Ta0.2Nb0.8)O3 with 2 wt % MnO2 addition (KNNLT-M) film on the transparent La0.03Ba0.97SnO3-coated LaAlO3 (001) substrate is chosen to investigate how the lattice evolution, as well as the electrical properties, optical bandgap energy, and thermal stability, changes with the growth oxygen pressure [P(O2)]. Compared to the other perovskite oxide films, for example, (La,Ca)MnO3, PbTiO3, and BaTiO3, an anomalous lattice evolution with an increased (decreased) out-of-plane (in-plane) lattice constant was observed in KNNLT-M films as P(O2) increases. Such anomalous lattice evolution can improve the electric properties of KNNLT-M films; for example, the ferroelectricity is significantly optimized and the dielectric constant is enhanced from 451 to 1248 at 1 kHz. The X-ray photoelectron spectra results have demonstrated that high P(O2) can make more K cations to enter the perovskite lattice and the Mn2+/Mn3+ existing in KNNLT can effectively suppress the leakage behavior, thus promoting the electrical nature of KNNLT-M films. The optical measurements show that the KNNLT-M film heterostructures are highly transparent with a maximum transmittance of ∼80%, and both direct and indirect bandgap energies increase with increasing P(O2). Meanwhile, all these KNNLT-M films exhibit good thermal stability with stable ferroelectricity up to the high temperature of at least 125 °C. These results demonstrate that the control of the lattice structure and electrical properties by P(O2) is one of the important prerequisites for the application of KNN-based films.

Keywords: electrical properties; knnlt films; lattice evolution; anomalous lattice; lattice

Journal Title: Inorganic chemistry
Year Published: 2022

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