Camila da Costa Ribeiro, Alexander Tkach, Jacques Noudem, C. Randall, M. Elisabete Costa, Paula M. Vilarinho
Dielectric breakdown strength ( E bd ) limits the reliability and energy density of functional oxide ceramics in high-field applications. Here, we demonstrate that Spark Plasma Texturing (SPT) dramatically enhances E bd in Ba 0.6 Sr 0.4 TiO 3 (BST) ceramics. Dynamic thermo-mechanical coupling during SPT produces a near-fully dense, highly homogeneous microstructure with ultra-fine grains (0.44 μm), resulting in E bd of up to 515 kV·cm −1 , which is more than twice higher than 200 kV·cm −1 for conventionally sintered ceramics and one third higher than 384 kV·cm −1 for ceramics prepared by standard SPS. This enhancement is of extrinsic origin and grain-boundary-controlled: impedance spectroscopy reveals elevated activation energies and resistive grain-boundary barriers that suppress long-range charge migration, while the intrinsic electronic structure with bandgap ~ 3.0 eV remains unchanged. SPT is thus established as an effective route for grain-boundary engineering in functional oxides, enabling high-reliability energy storage and tunable radio-frequency devices.