Accurate optical spectra through time-dependent density functional theory based on screening-dependent hybrid functionals

Abstract

We investigate optical absorption spectra obtained through time-dependent density functional theory (TD-DFT) based on nonempirical hybrid functionals that are designed to correctly reproduce the dielectric function. The comparison with state-of-the-art $GW$ calculations followed by the solution of the Bethe-Sapeter equation (BSE-$GW$) shows close agreement for both the transition energies and the main features of the spectra. We confront TD-DFT with BSE-$GW$ by focusing on the model dielectric function and the local exchange-correlation kernel. The present TD-DFT approach achieves the accuracy of BSE-$GW$ at a fraction of the computational cost.

References in corpus (15)

• The GW method
• Progress in Time-Dependent Density-Functional Theory
• Ab initio calculation of excitonic effects in the optical spectra of semiconductors
• Role of Polar Phonons in the Photo Excited State of Metal Halide Perovskites
• 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
• Bound excitons in time-dependent density-functional-theory: optical and energy-loss spectra
• Dynamical excitonic effects in metals and semiconductors
• Comparing electron-phonon coupling strength in diamond, silicon and silicon carbide: First-principles study
• Quasiparticles and phonon satellites in spectral functions of semiconductors and insulators: Cumulants applied to full first principles theory and Fröhlich polaron
• Correlation energy for the homogeneous electron gas: exact Bethe-Salpeter solution and new approximate evaluation
• Assessing model-dielectric-dependent hybrid functionals on the antiferromagnetic transition-metal monoxides MnO, FeO, CoO, and NiO
• Lattice polarization effects on the screened Coulomb interaction $W$ of the GW approximation
• Beyond time-dependent exact-exchange: the need for long-range correlation
• Koopmans Meets Bethe-Salpeter: Excitonic Optical Spectra without GW

Cited by in corpus (16)

• Band gaps of crystalline solids from Wannier-localization based optimal tuning of a screened range-separated hybrid functional
• Excited state properties of point defects in semiconductors and insulators investigated with time-dependent density functional theory
• 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
• Self-Trapped Excitons in Metal-Halide Perovskites Investigated by Time-Dependent Density Functional Theory
• Multi-phonon diffuse scattering in solids from first-principles: Application to layered crystals and 2D materials
• Transferable screened range-separated hybrid functionals for electronic and optical properties of van der Waals materials
• Direct, indirect, and self-trapped excitons in Cs${}_2$AgBiBr${}_6$
• Optical absorption spectra of metal oxides from time-dependent density functional theory and many-body perturbation theory based on optimally-tuned hybrid functionals
• A Snapshot of Time-Dependent Density-Functional Theory
• 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
• Optimized effective potentials from the random-phase approximation: Accuracy of the quasiparticle approximation
• 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
• Advancing excited-state properties of two-dimensional materials using a dielectric-dependent hybrid functional
• First-principles study of excitons in the optical spectra of silver chloride
• Exchange-Correlation Functionals in 2D Materials: Applications, Challenges, and Limitations