ABSTRACT 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 (Li 3 TaO 4 and Li 3 NbO 4 ), four perovskites (NaTaO 3 , NaNbO 3 , KTaO 3 , and KNbO 3 ), two cation‐deficient perovskites (Ba 5 Ta 4 O 15 and Ba 5 Nb 4 O 15 ), and a previously unreported pyrochlore‐type oxide, CsTa 2 O 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.
Du et al. (Wed,) studied this question.