Electronic structure and intrinsic dielectric polarization of defect-engineered rutile TiO2

Abstract

Experimental realization of colossal permittivity associated with intrinsic dielectric polarization of defect-engineered (Nb, In) co-doped rutile TiO₂ appears to be most suitable for microelectronics and solid-state device applications. Combining resonant photoemission spectroscopy, X-ray absorption spectroscopy, and density functional theory calculations, we here present a coherent understanding of electronic structure, in-gap defect states, doped electron localization, and their connection with macroscopic polarization for various doping configurations. Most often, conventional sample preparation conditions introduce in-gap states of Ti^3+δ character, limiting the maximum achievable intrinsic polarization value. Our understanding provides a pathway to enhance intrinsic polarization and minimize dielectric loss through suitable defect-engineering.