There has been much recent interest in a so-called “giant-dielectric phenomenon” displayed by an unusual cubic perovskite-type material, CaCu3Ti4O12; however, the origin of the high permittivity has been unclear [M. A. Subramanian, L. Dong, N. Duan, B. A. Reisner, and A. W. Sleight, J. Solid State Chem. 151, 323 (2000); C. C. Homes, T. Vogt, S. M. Shapiro, S. Wakimoto, and A. P. Ramirez, Science 293, 673 (2001); A. P. Ramirez, M. A. Subramanian, M. Gardel, G. Blumberg, D. Li, T. Vogt, and S. M. Shapiro, Solid State Commun. 115, 217 (2000)]. Impedance spectroscopy on CaCu3Ti4O12 ceramics demonstrates that they are electrically heterogeneous and consist of semiconducting grains with insulating grain boundaries. The giant-dielectric phenomenon is therefore attributed to a grain boundary (internal) barrier layer capacitance (IBLC) instead of an intrinsic property associated with the crystal structure. This barrier layer electrical microstructure with effective permittivity values in excess of 10 000 can be fabricated by single-step processing in air at ∼1100 °C. CaCu3Ti4O12 is an attractive option to the currently used BaTiO3-based materials which require complex, multistage processing routes to produce IBLCs of similar capacity.

The grain size dependence of the “giant dielectric effect” in CaCu3Ti4O12 ceramics (arising from a semiconducting grain/insulating grain boundary microstructure) has been revealed by impedance spectroscopy of ceramics sintered for 3 h (see Figure, left) and 24 h (see Figure, right); a rise in permittivity from 9000 to 280 000 was found. The easy‐to‐prepare CaCu3Ti4O12 is a hot candidate for ceramic capacitor applications.

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