Optical absorption spectra of metal oxides from time-dependent density functional theory and many-body perturbation theory based on optimally-tuned hybrid functionals

Abstract

Using both time-dependent density functional theory (TDDFT) and the ``single-shot" $GW$ plus Bethe-Salpeter equation ($GW$-BSE) approach, we compute optical band gaps and optical absorption spectra from first principles for eight common binary and ternary closed-shell metal oxides (MgO, Al${}_2$O${}_3$, CaO, TiO${}_2$, Cu${}_2$O, ZnO, BaSnO${}_3$, and BiVO${}_4$), based on the non-empirical Wannier-localized optimally-tuned screened range-separated hybrid functional. Overall, we find excellent agreement between our TDDFT and $GW$-BSE results and experiment, with a mean absolute error less than 0.4 eV, including for Cu${}_2$O and ZnO, traditionally considered to be challenging for both methods.

References in corpus (61)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Optimized norm-conserving Vanderbilt pseudopotentials
• The PseudoDojo: Training and grading a 85 element optimized norm-conserving pseudopotential table
• Quantum ESPRESSO toward the exascale
• Perspective on density functional theory
• Electron-phonon interactions from first principles
• Localization and delocalization errors in density functional theory and implications for band-gap prediction
• BerkeleyGW: A Massively Parallel Computer Package for the Calculation of the Quasiparticle and Optical Properties of Materials and Nanostructures
• Quasiparticle Self-Consistent GW Theory
• All-electron self-consistent GW approximation: Application to Si, MnO, and NiO
• Quasiparticle band structure based on a generalized Kohn-Sham scheme
• Fundamental gaps of finite systems from the eigenvalues of a generalized Kohn-Sham method
• Quasiparticle self-consistent $GW$ method; a basis for the independent-particle approximation
• First-principles GW calculations for fullerenes, porphyrins, phtalocyanine, and other molecules of interest for organic photovoltaic applications
• The GW compendium: A practical guide to theoretical photoemission spectroscopy
• Giant Rydberg Excitons in Cuprous Oxide
• Excitonic effects in solids described by time-dependent density functional theory
• Combining GW calculations with exact-exchange density-functional theory: An analysis of valence-band photoemission for compound semiconductors
• Solid-state optical absorption from optimally-tuned time-dependent range-separated hybrid density functional theory
• One-shot calculation of temperature-dependent optical spectra and phonon-induced band-gap renormalization
• Quasiparticle and Optical Properties of Rutile and Anatase TiO${}_2$
• Quasiparticle and Optical Spectroscopy of Organic Semiconductors Pentacene and PTCDA from First Principles
• All-electron GW calculation based on the LAPW method: application to wurtzite ZnO
• A Benchmark of GW Methods for Azabenzenes: Is the GW Approximation Good Enough?
• Coulomb-hole summations and energies for GW calculations with limited number of empty orbitals: a modified static remainder approach
• Electronic structure and phase stability of oxide semiconductors: Performance of dielectric-dependent hybrid functional DFT, benchmarked against $GW$ band structure calculations and experiments
• Cubic scaling $GW$: towards fast quasiparticle calculations
• Adequacy of Approximations in GW Theory
• Localized Orbital Scaling Correction for Systematic Elimination of Delocalization Error in Density Functional Approximations
• Effect of Semicore Orbitals on the Electronic Band Gaps of Si, Ge, and GaAs within the GW Approximation
• The long-wavelength behaviour of the exchange-correlation kernel in the Kohn-Sham theory of periodic systems
• Theory of the special displacement method for electronic structure calculations at finite temperature
• Predominance of non-adiabatic effects in zero-point renormalization of the electronic band gap
• Band gaps of crystalline solids from Wannier-localization based optimal tuning of a screened range-separated hybrid functional
• Phonon Screening of Excitons in Semiconductors: Halide Perovskites and Beyond
• Fundamental gaps with approximate density functionals: the derivative discontinuity revealed from ensemble considerations
• Beyond the quasiparticle approximation: Fully self-consistent $GW$ calculations
• Experimental and theoretical electronic structure of quinacridone
• Systematic beyond-DFT study of binary transition metal oxides
• Automation methodologies and large-scale validation for $GW$, towards high-throughput $GW$ calculations
• Accurate optical spectra through time-dependent density functional theory based on screening-dependent hybrid functionals
• Towards predictive band gaps for halide perovskites: Lessons from one-shot and eigenvalue self-consistent GW
• Koopmans-compliant spectral functionals for extended systems
• Theory of defects in one-dimensional systems: the case of Al in Si nanowires
• Reproducibility in $G_0{W}_0$ Calculations for Solids
• Accurate and efficient band-gap predictions for metal halide perovskites at finite temperature
• Assessing model-dielectric-dependent hybrid functionals on the antiferromagnetic transition-metal monoxides MnO, FeO, CoO, and NiO
• Deviations from piecewise linearity in the solid-state limit with approximate density functionals
• Zero-point Renormalization of the Band Gap of Semiconductors and Insulators Using the PAW Method
• An Optimally-Tuned Starting Point for Single-Shot $GW$ Calculations of Solids
• Koopmans Meets Bethe-Salpeter: Excitonic Optical Spectra without GW
• Optical properties of CsCu${}_2$X${}_3$ (X=Cl, Br and I): A comparative study between hybrid time-dependent density-functional theory and the Bethe-Salpeter equation
• Transition state method and Wannier functions
• koopmans: an open-source package for accurately and efficiently predicting spectral properties with Koopmans functionals
• Transferable screened range-separated hybrid functionals for electronic and optical properties of van der Waals materials
• Bloch's theorem in orbital-density-dependent functionals: Band structures from Koopmans spectral functionals
• Accurate optical spectra of solids from pure time-dependent density-functional theory
• A consistent picture of excitations in cubic BaSnO${}_3$ revealed by combining theory and experiment
• Localized orbital scaling correction for periodic systems
• Insights and challenges of applying the $GW$ method to transition metal oxides

Cited by in corpus (6)

• The reliability of hybrid functionals for accurate fundamental and optical gap prediction of bulk solids and surfaces
• Electronic structure and optical properties of halide double perovskites from a Wannier-localized optimally-tuned screened range-separated hybrid functional
• Compressing Hamiltonians with ab initio downfolding for simulating strongly-correlated materials on quantum computers
• Foundations of the ionization potential condition for localized electron removal in density functional theory
• Many-body perturbation theory with hybrid density functional theory starting points accelerated by adaptively compressed exchange
• Optical excitations in nanographenes from the Bethe-Salpeter equation and time-dependent density functional theory: absorption spectra and spatial descriptors