Entropy-driven charge redistribution for enhanced electromagnetic wave absorption in high-entropy single-atom materials

High-entropy single-atom (HE SAs), distinguished by maximized atomic utilization efficiency and tunable coordination geometries, represent a frontier in atomic-scale electromagnetic wave (EMW) absorber design. Nevertheless, precise HE SAs synthesis and atomic-level structure–absorption correlation mapping remain formidable challenges. Herein, we report an entropy-stabilization strategy to co-anchor multiple transition metals within a carbon matrix, concurrently suppressing atomic aggregation while engineering asymmetric charge distributions and enhanced electronic conductivity for superior EMW dissipation. Differential electronegativity and ionic radii among multimetallic sites induce localized asymmetric coordination environments, generating intensive electric dipole polarization centers. Synergistic multielement interactions further drive rapid interfacial charge redistribution and efficient electron transfer, significantly boosting conduction loss. The optimized HE SAs@CN system achieves exceptional EMW absorption: a minimal reflection loss of −76.8 dB at 8.57 GHz and a 5.00 GHz effective absorption bandwidth at 2.81 mm thickness, outperforming all benchmark single-metal analogs. This study establishes HE SA-doped carbon architectures as a paradigm for dielectric property modulation, providing fundamental insights into atomic-scale EMW loss mechanisms.