Regulation mechanism of negative permittivity in percolating composites via building blocks

Percolating composites with negative permittivity can be promising candidates for metamaterials; however, building blocks of negative permittivity have not yet been put forward in percolating composites. Here, the dielectric properties of a ternary composite with Fe and SiO2-coated Fe particles dispersed in a polymer matrix were investigated in the range of 10MHz-1GHz. By gradually controlling the Fe/coated-Fe ratio (x), a three-dimensional conductive network could be constructed when x exceeds 0.75. The Drude-type negative permittivity was achieved by the conductive network, and its Lorentz-type dispersion was mainly attributed to dielectric resonance of coated-Fe particles. Equivalent circuit analysis demonstrated that the inductive conductive network was the decisive building block to achieve negative permittivity. Moreover, the dielectric resonance caused by coated-Fe particles was LC resonance, and this indicated that the capacitive isolated metallic particles acted as another building block to control the dispersion of negative permittivity by LC resonance. Our reported work provides a highly efficient strategy to adjust negative permittivity and will facilitate applications of negative permittivity materials.