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Multi-component occupancies of perovskite materials (ABO3) have brought diverse crystallographic distortions and highly tunable defect structures. These structural features enable ABO3 to have customizable dielectric and magnetic properties, offering new opportunities for advancing microwave absorbing materials. In this study, entropy-driven strategies, including composition optimization, structural/defective design, microstructure engineering, and microwave absorption simulation, are proposed to improve the microwave absorption capacity of (Ba1/3Sr1/3Ca1/3)FeO3. The hexagonal perovskite structure (Ba1/3Sr1/3Ca1/3)FeO3 prepared at 1100 °C exhibits exceptional electromagnetic wave absorption properties, with a minimum reflection loss of −40.58 dB at a thickness of 1.2 mm and a maximum effective absorption bandwidth of 4.16 GHz. The results indicate that the interconnection of octahedra, and structural distortions, oxygen vacancies, and other defects enhance the dielectric polarization of the material, leading to excellent wave absorption performance. The entropy-driven design strategy for perovskite ABO3 materials offers valuable insights for the development of advanced electromagnetic wave absorption materials.
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