Multiple optical impacts of anion doping in epitaxial barium titanate films

Multiple strong impacts of anion doping Lambda (Lambda = oxygen vacancy, nitrogen, or hydrogen) on the optical properties in the near-infrared to vacuum ultraviolet spectral range are experimentally revealed in cube-on-cube-type epitaxial perovskite BaTiO3-delta Lambda (delta) films (delta <= 0.01) grown on (001)SrTiO3 substrates. Compared to the reference undoped films and bulk crystal, the anion-doped films exhibit massive changes of the index of refraction in the transparency range Delta n of similar to 0.1 to 0.2, a profound bandgap widening Delta E-g of similar to 0.3 eV to 0.4 eV, a dopant-specific near-edge absorption, and doping-induced interband transitions. Both the conduction-band uplift and the changes in the index of refraction are ascribed to the internal stress and electric field, which result from epitaxially controlled dopant locations in the [Ba-O](001) planes. The dopant-induced in-gap states are responsible for the near-edge absorption, whereas the dopant-induced conduction-band states are suggested to modify the interband transitions and the intrinsic elasto- and electro-optic coefficients.