Electronic and optical properties of doped TiO2 by many-body perturbation theory

Abstract

Doping is one of the most common strategies for improving the photocatalytic and solar energy conversion properties of TiO${}_2$, hence an accurate theoretical description of the electronic and optical properties of doped TiO${}_2$ is of both scientific and practical interest. In this work we use many-body perturbation theory techniques to investigate two typical n-type dopants, Niobium and Hydrogen, in TiO${}_2$ rutile. Using the GW approximation to determine band edges and defect energy levels, and the Bethe Salpeter equation for the calculation of the absorption spectra, we find that the defect energy levels form non-dispersive bands %associated with localized states lying $\simeq 2.2eV$ above the top of the corresponding valence bands ($\simeq 0.9eV$ below the conduction bands of the {\it pristine} material). The defect states are also responsible for the appearance of low energy absorption peaks that enhance the solar spectrum absorption of rutile. The spatial distributions of the excitonic wavefunctions associated with these low energy excitations are very different for the two dopants, suggesting a larger mobility of photoexcited electrons in Nb-TiO${}_2$.

arXiv comment8 pages, 6 figures

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• First-principles Hubbard U and Hund's J corrected approximate density-functional theory predicts an accurate fundamental gap in rutile and anatase TiO2
• Self energy and excitonic effect in (un)doped TiO${}_2$ anatase : A comparative study of hybrid DFT, GW and BSE to explore optical properties