Post density functional theoretical studies of highly polar semiconductive Pb(Ti${}_{1-x}$Ni${}_x$)O${}_{3-x}$ solid solutions: The effects of cation arrangement on band gap

Abstract

We use a combination of conventional density functional theory (DFT) and post-DFT methods, including the local density approximation plus Hubbard $U$ (LDA+$U$), PBE0, and self-consistent $GW$ to study the electronic properties of Ni-substituted PbTiO${}_3$ (Ni-PTO) solid solutions. We find that LDA calculations yield unreasonable band structures, especially for Ni-PTO solid solutions that contain an uninterrupted NiO${}_2$ layer. Accurate treatment of localized states in transition-metal oxides like Ni-PTO requires post-DFT methods. $B$-site Ni/Ti cation ordering is also investigated. The $B$-site cation arrangement alters the bonding between Ni and O, and therefore strongly affects the band gap ($E_{\mathrm{g}}$) of Ni-PTO. We predict that Ni-PTO solid solutions should have a direct band gap in the visible light energy range, with polarization similar to the parent PbTiO${}_3$. This combination of properties make Ni-PTO solid solutions promising candidate materials for solar energy conversion devices.

19 pages, 6 figures

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