Precisely tuning ε′-negative and ε′-near-zero responses by synergistic effect of graphene and carbon black in ternary metacomposites

Understanding how to precisely regulate the magnitude and dispersion characteristics of radio-frequency (RF) ε’-negative and ε’-near-zero (ENZ) responses presents a challenge. This challenge significantly impacts the design of versatile electronic devices. In this study, we introduce a synergistic strategy utilizing graphene (GR) and carbon black (CB) in ternary metacomposites for tunable ε’-negative and ENZ responses. Due to the randomly constructed 3-dimensional (3D) conductive GR-CB networks in a CaCu₃Ti₄O₁₂ matrix, we observed two types of ε’-negative response mechanisms: electric dipole resonance and low-frequency plasma oscillation, which dominate at different frequency bands. Consequently, the weakly ε’-negative values (0 < |ε’| 〈1000) and frequency dispersion were successfully adjusted due to the interplay between these two mechanisms. The ENZ frequencies were also tuned over ∼580 MHz, 225 MHz, ∼189 MHz and ∼ 188 MHz with variable GR-to-CB ratios. Furthermore, we studied the conduction behavior, loss mechanism, and electrical characteristics of the ε’-negative metacomposites to shed light on the relationship between microstructural changes and dielectric performance.