Intrinsic Piezoelectric Anisotropy of Tetragonal ABO3 Perovskites: A High-Throughput Study

Abstract: A comprehensive understand of the intrinsic piezoelectric anisotropy stemming from diverse chemical and physical factors is a key step for the rational design of highly anisotropic materials. We performed high-throughput calculations on tetragonal ABO3 perovskites to investigate the piezoelectricity and the interplay between lattice, displacement, polarization and elasticity. Among the 123 types of perovskites, the structural tetragonality is naturally divided into two categories: normal tetragonal (c/a ratio < 1.1) and super-tetragonal (c/a ratio > 1.17), exhibiting distinct ferroelectric, elastic, and piezoelectric properties. Charge analysis revealed the mechanisms underlying polarization saturation and piezoelectricity suppression in the super-tetragonal region, which also produces an inherent contradiction between high d33 and large piezoelectric anisotropy ratio |d33/d31|. The polarization axis and elastic softness direction jointly determine the maximum longitudinal piezoelectric response d33 direction. The validity and deficiencies of the widely utilized |d33/d31| ratio for representing piezoelectric anisotropy were reevaluated.