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

The epitaxial (K0.oa0.oi0.02)(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 degrees 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.