Structure characteristics and microwave/terahertz dielectric response of low-permittivity (La0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Zr3(MoO4)9 high-entropy ceramics

Abstract

Microwave dielectric ceramics play a vital role in wireless communication systems. However, it is a great challenge to obtain ideal performances of single-phase ceramics. In this work, (La0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Zr3(MoO4)9 (abbreviated as L5ZMO) high-entropy ceramics were successfully prepared by the solid-state reaction method, the pure trigonal L5ZMO structure can be synthesized in the mixture calcined at 700 °C. Rietveld refinement based on XRD data reveals that lattice parameters of L5ZMO ceramics are affected by the radius of the five rare earth elements, which indicates that the rare earth elements have been solubilized and randomly distributed in the Ln-site. The relative density illustrates a strong dependence on sintering temperature, which gradually increases with increasing sintering temperature. Based on the analysis of bond characteristics, the Mo–O bond exhibits a vital effect on the dielectric properties of L5ZMO ceramics. Besides, the infrared reflection spectrum and terahertz time-domain spectroscopy analysis show that ionic polarization is the dominant polarization in the microwave/terahertz bands. Meanwhile, the tan δ can be further reduced by optimizing process parameters. Notably, the L5ZMO high-entropy ceramics sintered at 750 °C exhibit outstanding dielectric properties of εr = 10.46, Q·f = 59,713 GHz, and τf = −21.94 ppm/°C, indicating that the high-entropy design optimizes τf (−38.8 ppm/°C) of the simple La2Zr3(MoO4)9 ceramics. The attempt provides theoretical guidance for the application of high-entropy design concepts in microwave/terahertz bands.