title: Self-Consistent Hybrid Functional Calculations: Implications for Structural, Electronic, and Optical Properties of Oxide Semiconductors.
abstract: The development of new exchange-correlation functionals within density functional theory means that increasingly accurate information is accessible at moderate computational cost. Recently, a newly developed self-consistent hybrid functional has been proposed (Skone et al., Phys. Rev. B 89:195112, 2014), which allows for a reliable and accurate calculation of material properties using a fully ab initio procedure. Here, we apply this new functional to wurtzite ZnO, rutile SnO2, and rocksalt MgO. We present calculated structural, electronic, and optical properties, which we compare to results obtained with the PBE and PBE0 functionals. For all semiconductors considered here, the self-consistent hybrid approach gives improved agreement with experimental structural data relative to the PBE0 hybrid functional for a moderate increase in computational cost, while avoiding the empiricism common to conventional hybrid functionals. The electronic properties are improved for ZnO and MgO, whereas for SnO2the PBE0 hybrid functional gives the best agreement with experimental data.
authors.affiliation: Department of Chemistry, University of Bath, Claverton Down, BA2 7AY, Bath, UK. d.fritsch@bath.ac.uk.
authors.forename: Daniel
authors.identifier: http://orcid.org/0000-0003-4708-2456
authors.initials: D
authors.lastname: Fritsch
authors.affiliation: Department of Chemistry, University of Bath, Claverton Down, BA2 7AY, Bath, UK.
authors.forename: Benjamin J
authors.initials: BJ
authors.lastname: Morgan
authors.affiliation: Department of Chemistry, University of Bath, Claverton Down, BA2 7AY, Bath, UK.
authors.forename: Aron
authors.initials: A
authors.lastname: Walsh
keywords: Density functional theory; Dielectric functions; Hybrid functionals; Semiconducting oxides