Geometry-defect-spin coupling in chiral high-entropy systems: Multiscale mechanisms of GHz electromagnetic...

Chiral electromagnetic materials, with their unique spatial configurations, can regulate the propagation and polarization of electromagnetic waves, serving as powerful tools for tailoring electromagnetic behavior. However, their functional potential is often limited by the intrinsic constraints of conventional host materials, which typically lack sufficient flexibility in defect engineering, magnetic modulation, and spin-orbit coupling (SOC) enhancement. To address this challenge, we introduce high-entropy metal oxides (HEMOs) into carbon-based chiral frameworks, constructing HEMO and carbon nanocoil (HEMO@CNC) composites. By combining advanced microscopy, electromagnetic measurements, and density functional theory (DFT) calculations, it is revealed that increasing entropy and helical strain jointly induce nonlinear changes in SOC strength and defect-related localized states. Benefiting from these effects, the HEMO@CNC system achieves an ultrawide bandwidth, outperforming linear structures and low-entropy systems. This work provides a potential paradigm for integrating topological defect engineering and high-entropy quantum modulation, offering deeper insights into advancing electromagnetic functional materials from macroscopic design toward geometry-defect-spin synergistic regulation.