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The development of dielectric materials with colossal permittivity isimportant for the miniaturization of electronic devices and fabrication ofhigh-density energy-storage devices. The electron-pinned defect-dipoles hasbeen recently proposed to boost the permittivity of (Nb + In) co-doped TiO2 to105. However, the follow-up studies suggest an extrinsic contribution to thecolossal permittivity from thermally excited carriers. Herein, we demonstrate amarked enhancement in the permittivity of (Nb + In) co-doped TiO2 singlecrystals at sufficiently low temperatures such that the thermally excitedcarriers are frozen out and exert no influence on the dielectric response. Theresults indicate that the permittivity attains quadruple of that for pure TiO2.This finding suggests that the electron-pinned defect-dipoles add an extradielectric response to that of the TiO2 host matrix. The results offer a novelapproach for the development of functional dielectric materials with largepermittivity by engineering complex defects into bulk materials.

Intrinsic Enhancement of Dielectric Permittivity in (Nb + In) co-doped TiO2 single crystals