Multiscale Structural Modulation and Synergistic Enhancement of Transparency and Relaxor Behavior in La³⁺-Doped KNN...

Lead-free transparent ferroelectric ceramics with integrated opto-electro-mechanical functionalities are pivotal for next-generation multifunctional devices. In this study, K_0.48Na_0.52NbO₃-xLa₂O₃ (KNN-xLa, x = 0.005 - 0.04) ceramics were fabricated via a conventional solid-state route to investigate the La³⁺-induced multiscale structural evolution and its modulation of optical and electrical properties. La³⁺ substitution drives a critical structural transition from an anisotropic orthorhombic phase (Amm2) to a high-symmetry pseudocubic-like tetragonal phase (P4mm) for x ≥ 0.025, characterized by minimal lattice distortion (c/a = 1.0052). This enhanced structural isotropy, coupled with submicron grain refinement (<1 μm) driven by VA'-mediated solute drag, effectively suppresses light scattering. Consequently, a high-transparency plateau (T₇₈₀ ≈ 53-58%, T₁₇₀₀ ≈ 70-72%) is achieved for 0.025 ≤ x ≤ 0.035. Simultaneously, the system undergoes a crossover from normal ferroelectric (FE) to relaxor (RF) state, governed by an FE-RF boundary at x = 0.015. While x = 0.005 exhibits robust piezoelectricity (d₃₃ ≈ 92 pC/N), the x = 0.015 composition facilitates a transitional polar state with large strain (0.179%) and high polarization (P_m ≈ 33.3 μC/cm², P_r ≈ 15.8 μC/cm²). Piezoresponse force microscopy (PFM) confirms the domain evolution from lamellar macro-domains to speckle-like polar nanoregions (PNRs), elucidating the intrinsic trade-off between optical transparency and piezoelectricity. This work underscores La³⁺ as a potent structural modifier for tailoring phase boundaries and defect chemistry, providing a cost-effective framework for developing high-performance transparent electromechanical materials.