Theory-Guided Exploration of the Sr2Nb2O7 System for Increased Dielectric and Piezoelectric Properties and Synthesis of Vanadium-Alloyed Sr2Nb2O7

Ab initio methods provide a powerful tool in the search for novel polar materials. In particular, there has been a surge to identify lead-free piezoelectric materials to replace PbZr0.52Ti0.48O3. This study examines a computational strategy to identify increased piezoelectric and dielectric responses of alloy systems based on the linear interpolation of force constants, Born effective charges, and internal strain tensors from their end-point compounds. We choose the ferroelectric layered perovskite Sr2Nb2O7 as a parent structure and employ this alloying strategy for 19 potential cation substitutions, targeting thermodynamically metastable alloys with high piezoelectric response. From this screening, we identify Sr2Nb2–2xV2xO7 as a promising polar system. We conduct large-unit-cell calculations of Sr2Nb2–2xV2xO7 at x = 0.0625, 0.125 for multiple cation orderings and find a significant 184% enhanced piezoelectric response. The solid solution system is synthesized as single-crystalline thin-film heterostructures using pulsed-laser deposition, and an enhanced dielectric response is observed at x = 0.05 and at x = 0.1. We present the Sr2Nb2–2xV2xO7 alloy system designed through high-throughput computational screening methods with a large calculated piezoelectric response and experimentally verified increased dielectric response. Our methodology is provided as a high-throughput screening tool for novel materials with enhanced polarizability and alloy systems with potential morphotropic phase boundaries.