Flexoelectric Polarization Enhancement in Paraelectric BaHfO ₃ via Strain Gradient Engineering

Abstract Flexoelectricity – polarization induced by strain gradients – offers a route to polar functionality in centrosymmetric dielectrics, where traditional piezoelectric effects are absent. This study investigates the flexoelectric effect in epitaxial BaHfO ₃ (BHO) thin films, a centrosymmetric and paraelectric perovskite. While a large lattice mismatch induces defect‐driven relaxation, a coherently grown BHO film undergoes elastic relaxation, forming intrinsic strain gradients exceeding 10 ⁵ m ⁻¹ . A 29‐fold enhancement in spontaneous polarization is observed at an electric field of 4 MV cm ⁻¹ for BHO exhibiting a strain gradient compared to relaxed BHO. This enhancement is attributed to flexoelectric coupling, which is isolated from ferroelectric and piezoelectric contributions due to the centrosymmetric nature and the absence of phase transitions in BHO. The findings establish a clear link between engineered strain gradients and enhanced polarizability in oxide thin films, offering a benchmark system for deconvoluting the flexoelectric effect from other polar effects. These results provide a basis for exploiting flexoelectricity in dielectric devices and advance the fundamental understanding of strain‐coupled phenomena in functional oxides.