Band gaps of crystalline solids from Wannier-localization based optimal tuning of a screened range-separated hybrid functional

Abstract

Accurate prediction of fundamental band gaps of crystalline solid state systems entirely within density functional theory is a long standing challenge. Here, we present a simple and inexpensive method that achieves this by means of non-empirical optimal tuning of the parameters of a screened range-separated hybrid functional. The tuning involves the enforcement of an ansatz that generalizes the ionization potential theorem to the removal of an electron in an occupied state described by a localized Wannier function in a modestly sized supercell calculation. The method is benchmarked against experiment for a set of systems ranging from narrow band gap semiconductors to large band gap insulators, spanning a range of fundamental band gaps from 0.2 to 14.2 eV and is found to yield quantitative accuracy across the board, with a mean absolute error of $\sim$0.1 eV and a maximal error of $\sim$0.2 eV.

10 pages, 2 figures

References in corpus (10)

• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Localization and delocalization errors in density functional theory and implications for band-gap prediction
• An approximation to density functional theory for an accurate calculation of band-gaps of semiconductors
• Self-consistent hybrid functional for condensed systems
• The GW compendium: A practical guide to theoretical photoemission spectroscopy
• Localized Orbital Scaling Correction for Systematic Elimination of Delocalization Error in Density Functional Approximations
• Automation methodologies and large-scale validation for $GW$, towards high-throughput $GW$ calculations
• Enhanced Static Approximation to the Electron Self-Energy Operator for Efficient Calculation of Quasiparticle Energies
• Deviations from piecewise linearity in the solid-state limit with approximate density functionals
• 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

Cited by in corpus (31)

• Extensive Benchmarking of DFT+U Calculations for Predicting Band Gaps
• Theory of Cross Phenomena and Their Coefficients Beyond Onsager Theorem
• The quantum geometric origin of capacitance in insulators
• Accurate electronic properties and intercalation voltages of olivine-type Li-ion cathode materials from extended Hubbard functionals
• An Optimally-Tuned Starting Point for Single-Shot $GW$ Calculations of Solids
• Importance of intersite Hubbard interactions in $\beta$-MnO${}_2$: A first-principles DFT+$U$+$V$ study
• 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
• The Wannier Function Software Ecosystem for Materials Simulations
• Bloch's theorem in orbital-density-dependent functionals: Band structures from Koopmans spectral functionals
• Accurate non-empirical range-separated hybrid van der Waals density functional for complex molecular problems, solids, and surfaces
• Optical absorption spectra of metal oxides from time-dependent density functional theory and many-body perturbation theory based on optimally-tuned hybrid functionals
• Localized orbital scaling correction for periodic systems
• On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS${}_3$ and CrI${}_3$
• Hybridization driving distortions and multiferroicity in rare-earth nickelates
• Addressing the Band Gap Problem with a Machine-Learned Exchange Functional
• A general framework for active space embedding methods: applications in quantum computing
• Embedding vertex corrections in GW self-energy: theory, implementation, and outlook
• The reliability of hybrid functionals for accurate fundamental and optical gap prediction of bulk solids and surfaces
• Native point defects in HgCdTe infrared detector material: Identifying deep centers from first principles
• Electronic structure and optical properties of halide double perovskites from a Wannier-localized optimally-tuned screened range-separated hybrid functional
• Magnons from time-dependent density-functional perturbation theory and nonempirical Hubbard functionals
• State-specific density functionals for excited states from ensembles
• Compressing Hamiltonians with ab initio downfolding for simulating strongly-correlated materials on quantum computers
• Spin-dependent interactions in orbital-density-dependent functionals: non-collinear Koopmans spectral functionals
• Predicting electronic screening for fast Koopmans spectral functional calculations
• Correcting Delocalization Error in Materials with Localized Orbitals and Linear-Response Screening
• Foundations of the ionization potential condition for localized electron removal in density functional theory
• Comparison of long-range corrected kernels and range-separated hybrids for excitons in solids
• Wannier Functions Dually Localized in Space and Energy
• Many-body perturbation theory with hybrid density functional theory starting points accelerated by adaptively compressed exchange