Automation methodologies and large-scale validation for $GW$, towards high-throughput $GW$ calculations

Abstract

The search for new materials, based on computational screening, relies on methods that accurately predict, in an automatic manner, total energy, atomic-scale geometries, and other fundamental characteristics of materials. Many technologically important material properties directly stem from the electronic structure of a material, but the usual workhorse for total energies, namely density-functional theory, is plagued by fundamental shortcomings and errors from approximate exchange-correlation functionals in its prediction of the electronic structure. At variance, the $GW$ method is currently the state-of-the-art {\em ab initio} approach for accurate electronic structure. It is mostly used to perturbatively correct density-functional theory results, but is however computationally demanding and also requires expert knowledge to give accurate results. Accordingly, it is not presently used in high-throughput screening: fully automatized algorithms for setting up the calculations and determining convergence are lacking. In this work we develop such a method and, as a first application, use it to validate the accuracy of $G_0{W}_0$ using the PBE starting point, and the Godby-Needs plasmon pole model ($G_0{W}_0^{\text{GN}}$@PBE), on a set of about 80 solids. The results of the automatic convergence study utilized provides valuable insights. Indeed, we find correlations between computational parameters that can be used to further improve the automatization of $GW$ calculations. Moreover, we find that $G_0{W}_0^{\text{GN}}$@PBE shows a correlation between the PBE and the $G_0{W}_0^{\text{GN}}$@PBE gaps that is much stronger than that between $GW$ and experimental gaps. However, the $G_0{W}_0^{\text{GN}}$@PBE gaps still describe the experimental gaps more accurately than a linear model based on the PBE gaps.

12 pages, 11 figures

References in corpus (28)

• Optimized norm-conserving Vanderbilt pseudopotentials
• The GW method
• Yambo: an \textit{ab initio} tool for excited state calculations
• BerkeleyGW: A Massively Parallel Computer Package for the Calculation of the Quasiparticle and Optical Properties of Materials and Nanostructures
• Quasiparticle Self-Consistent GW Theory
• Resolution-of-identity approach to Hartree-Fock, hybrid density functionals, RPA, MP2, and \textit{GW} with numeric atom-centered orbital basis functions
• Random-phase approximation and its applications in computational chemistry and materials science
• All-electron self-consistent GW approximation: Application to Si, MnO, and NiO
• Quasiparticle band structure based on a generalized Kohn-Sham scheme
• Combining GW calculations with exact-exchange density-functional theory: An analysis of valence-band photoemission for compound semiconductors
• Unified description of ground and excited states of finite systems: the self-consistent GW approach
• A Benchmark of GW Methods for Azabenzenes: Is the GW Approximation Good Enough?
• All-electron GW calculation based on the LAPW method: application to wurtzite ZnO
• Predictive GW calculations using plane waves and pseudopotentials
• The GW space-time method for the self-energy of large systems
• Band convergence and linearization error correction of all-electron GW calculations: The extreme case of zinc oxide
• Quasi-Particle Self-Consistent $GW$ for Molecules
• Benchmark of GW approaches for the GW100 testset
• Band widths and gaps from the Tran-Blaha functional : Comparison with many-body perturbation theory
• Dynamical and anharmonic effects on the electron-phonon coupling and the zero-point renormalization of the electronic structure
• The bandstructure of gold from many-body perturbation theory
• Electronic structure of Pu and Am metals by self consistent relativistic GW
• Accurate all-electron $G_0{W}_0$ quasiparticle energies employing the full-potential augmented planewave method
• Elimination of the linearization error in GW calculations based on the linearized augmented-plane-wave method
• Towards Fully Converged GW Calculations for Large Systems
• Piecewise linearity in the $GW$ approximation for accurate quasiparticle energy predictions
• First-principles calculation of electronic excitations in solids with SPEX
• Ab-initio self-energy corrections in systems with metallic screening

Cited by in corpus (22)

• The PseudoDojo: Training and grading a 85 element optimized norm-conserving pseudopotential table
• The GW compendium: A practical guide to theoretical photoemission spectroscopy
• Band gaps of crystalline solids from Wannier-localization based optimal tuning of a screened range-separated hybrid functional
• MODNet -- accurate and interpretable property predictions for limited materials datasets by feature selection and joint-learning
• Roadmap on Electronic Structure Codes in the Exascale Era
• All-electron Gaussian-based $G_0{W}_0$ for Valence and Core Excitation Energies of Periodic Systems
• Converged GW quasiparticle energies for transition metal oxide perovskites
• Accurate electronic band gaps of two-dimensional materials from the local modified Becke-Johnson potential
• Computational Search for Magnetic and Non-magnetic 2D Topological Materials using Unified Spin-orbit Spillage Screening
• An Optimally-Tuned Starting Point for Single-Shot $GW$ Calculations of Solids
• Relativistic Self-Consistent $GW$: Exact Two-Component Formalism with One-Electron Approximation for Solids
• Cubic BN optical gap and intragap optically active defects
• Computationally-driven, high throughput identification of CaTe and Li${}_{\text{3}}$Sb as promising candidates for high mobility $p$-type transparent conducting materials
• Abinit 2025: New Capabilities for the Predictive Modeling of Solids and Nanomaterials
• Electronic Band Structure of Cuprous and Silver Halides: a Numerically Accurate All-Electron $GW$ Study
• Convergence and pitfalls of density functional perturbation theory phonons calculations from a high-throughput perspective
• Optical absorption spectra of metal oxides from time-dependent density functional theory and many-body perturbation theory based on optimally-tuned hybrid functionals
• Delocalization of dark and bright excitons in flat-band materials and the optical properties of V${}_2$O${}_5$
• Towards high-throughput many-body perturbation theory: efficient algorithms and automated workflows
• Verification and Validation of zero-point electron-phonon renormalization of the bandgap, mass enhancement, and spectral functions
• Electronic structure and optical properties of halide double perovskites from a Wannier-localized optimally-tuned screened range-separated hybrid functional
• First-principles study of excitons in the optical spectra of silver chloride