Accelerated Oxide Materials Discovery Through High-Throughput Synthesis and Characterization

Complex oxides host diverse physical phenomena and multifunctional responses, making them central to next-generation information storage, energy conversion, and smart sensing technologies. Among them, pyrochlore dielectrics, characterized by moderate permittivity and low hysteresis loss, are attractive candidates for high-energy-density capacitors. However, conventional trial-and-error strategies for exploring complex oxide phase space remain time-consuming and inefficient, limiting materials discovery. Here, we establish a high-throughput combinatorial workflow that integrates accelerated hydrothermal synthesis, droplet-based transmission electron microscopy sample preparation, and multi-modal phase characterization. Screening sixteen compositional variants resulted in nine distinct phases, including two ion-conducting oxides (Li₃TaO₄ and Li₃NbO₄), four perovskites (NaTaO₃, NaNbO₃, KTaO₃, and KNbO₃), two cation-deficient perovskites (Ba₅Ta₄O₁₅ and Ba₅Nb₄O₁₅), and a previously unreported pyrochlore-type oxide, CsTa₂O_6-X. Atomic-resolution scanning transmission electron microscopy resolves its structural framework, while measurements from a ferroelectric analyzer demonstrate that its dielectric energy storage performance is on par with that of advanced paraelectric or linear dielectric ceramics, with an efficiency of 96.5%. Collectively, this work demonstrates an accelerated discovery paradigm for functional oxides by coupling high-throughput hydrothermal phase screening, automated sample preparation and structural characterization, and cross-scale structure-property correlation, providing a scalable route toward rapid exploration of complex oxide materials.