Defect calculations in semiconductors through a dielectric-dependent hybrid DFT functional: the case of oxygen vacancies in metal oxides

Abstract

We investigate the behavior of oxygen vacancies in three different metal-oxide semiconductors (rutile and anatase TiO2, monoclinic WO3, and tetragonal ZrO2) using a recently proposed hybrid density-functional method in which the fraction of exact exchange is material-dependent but obtained ab initio in a self-consistent scheme. In particular, we calculate charge-transition levels relative to the oxygen-vacancy defect and compare computed optical and thermal excitation/emission energies with the available experimental results, shedding light on the underlying excitation mechanisms and related materials properties. We find that this novel approach is able to reproduce not only ground-state properties and band structures of perfect bulk oxide materials, but also provides results consistent with the optical and electrical behavior observed in the corresponding substoichiometric defective systems.

Accepted for publication in J. Chem. Phys

References in corpus (5)

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Cited by in corpus (9)

• Nonempirical Range-separated Hybrid Functionals for Solids and Molecules
• Band gaps of crystalline solids from Wannier-localization based optimal tuning of a screened range-separated hybrid functional
• Anisotropic Effects of Oxygen Vacancies on Electrochromic Properties and Conductivity of $\gamma$-Monoclinic WO${}_3$
• Dielectric dependent hybrid functionals for heterogeneous materials
• Assessing model-dielectric-dependent hybrid functionals on the antiferromagnetic transition-metal monoxides MnO, FeO, CoO, and NiO
• Factors determining surface oxygen vacancy formation energy in ternary spinel structure oxides with zinc
• Density functional descriptions of interfacial electronic structure
• Accurate and efficient prediction of the band gaps and optical spectra of chalcopyrite semiconductors from a non-empirical range-separated dielectric-dependent hybrid: Comparison with many-body perturbation theory
• Advancing excited-state properties of two-dimensional materials using a dielectric-dependent hybrid functional