Electronic structure and phase stability of oxide semiconductors: Performance of dielectric-dependent hybrid functional DFT, benchmarked against $GW$ band structure calculations and experiments

Abstract

We investigate band gaps, equilibrium structures, and phase stabilities of several bulk polymorphs of wide-gap oxide semiconductors ZnO, TiO2,ZrO2, and WO3. We are particularly concerned with assessing the performance of hybrid functionals built with the fraction of Hartree-Fock exact exchange obtained from the computed electronic dielectric constant of the material. We provide comparison with more standard density-functional theory and GW methods. We finally analyze the chemical reduction of TiO2 into Ti2O3, involving a change in oxide stoichiometry. We show that the dielectric-dependent hybrid functional is generally good at reproducing both ground-state (lattice constants, phase stability sequences, and reaction energies) and excited-state (photoemission gaps) properties within a single, fully ab initio framework.

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References in corpus (8)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Quasiparticle band structure based on a generalized Kohn-Sham scheme
• Self-consistent hybrid functional for condensed systems
• The stability, electronic structure, and optical property of TiO2 polymorphs
• Band Offsets at Semiconductor-Oxide Interfaces from Hybrid Density Functional Calculations
• Quasiparticle and Optical Properties of Rutile and Anatase TiO${}_2$
• Band convergence and linearization error correction of all-electron GW calculations: The extreme case of zinc oxide
• GW quasiparticle bandgaps of anatase TiO2 starting from DFT+U

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