Enhanced Electromagnetic Wave Absorption in Mapbi3 Hybrid Perovskite Through a Defect‐Tunable Green Synthesis

Defect engineering and structure‐property relationship understanding in methylammonium lead iodide (MAPI) hybrid perovskites (HPs) attract significant scientific interest, as synthesis‐related defects may strongly influence intrinsic properties. We have explored a green solvent‐free synthesis—mechanosynthesis—leading to large quantities of MAPI powder with tuneable defect density suitable to study MAPI as an electromagnetic wave absorbing (EMWA) material. A dielectric loss enhancement was revealed at 11.4 GHz (X‐band) for 4 h‐ground MAPI powders (MAPI4h), compared to 30 min‐ground powders (MAPI30) when the particle size was <20 μm. MAPI powders display a fractal microstructure with agglomerates of clusters of (nano)grains (≈80 nm for MAPI4h), consisting further of oriented smaller nanograin (5–10 nm) clusters. A strong reabsorption in smaller particles was evidenced due to a surface‐defective layer. MAPI4h was shown to display a more surface‐defective layer with a higher defect density gradient from surface to (nano)grains core and unique open defects different from those in solution‐processed MAPI. These vacancy‐type surface defects would enhance dipole polarization by stabilizing methylammonium dipoles, thereby increasing permittivity. The improved dispersion of MAPI particles (<20 μm) in polymeric matrixes enhanced the surface effects and effective interactions with electromagnetic waves. This study demonstrated the potential of this green synthesis for producing large amount of HPs and tuning defects, opening new avenues for HPs EMWA application.