All-electron Quasiparticle Self-consistent GW for Molecules and Periodic Systems within the Numerical Atomic Orbital Framework

Abstract

We report an all-electron implementation of the quasiparticle self-consistent GW (QSGW) method for molecular and periodic systems within the framework of numerical atomic orbitals (NAOs), as implemented in the LibRPA software package. Our implementation is based on the space-time formalism, combined with the localized resolution-of-identity approximation to treat two-electron quantities. We found that analytical continuation of the self-energy matrix, in combination with the ``Mode B" QSGW scheme, can yield stable self-consistent quasiparticle energy spectra. Systematic benchmark calculations on molecules and crystalline solids (including typical semiconductors and wide-gap insulators) demonstrate that our NAO-based QSGW scheme yields molecular ionization potentials and quasiparticle band gaps for periodic solids that are consistent with reference results from established implementations. Our work opens the way for large-scale QSGW calculations, taking advantage of the NAO-based low-scaling algorithm previously developed for the G0W0 method.

References in corpus (46)

• Electronic Structure Calculations with Dynamical Mean-Field Theory: A Spectral Density Functional Approach
• 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
• All-electron self-consistent GW approximation: Application to Si, MnO, and NiO
• Quasiparticle self-consistent $GW$ method; a basis for the independent-particle approximation
• The GW compendium: A practical guide to theoretical photoemission spectroscopy
• First principles approach to the electronic structure of strongly correlated systems: combining GW and DMFT
• Combining GW calculations with exact-exchange density-functional theory: An analysis of valence-band photoemission for compound semiconductors
• Fully selfconsistent GW calculations for molecules
• 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?
• The Band-Gap Problem in Semiconductors Revisited: Effects of Core States and Many-Body Self-Consistency
• Band convergence and linearization error correction of all-electron GW calculations: The extreme case of zinc oxide
• Self-consistent GW: All-electron implementation with localized basis functions
• Quasi-Particle Self-Consistent $GW$ for Molecules
• Benchmark of GW approaches for the GW100 testset
• Fully self-consistent GW calculations for atoms and molecules
• Hybrid-functional calculations with plane-wave basis sets: The effect of the singularity correction on total energies, energy eigenvalues, and defect energy levels
• Fully self-consistent $GW$ and quasi-particle self-consistent $GW$ for molecules
• Electronic structure of Na, K, Si, and LiF from self-consistent solution of Hedin's equations including vertex corrections
• Beyond the quasiparticle approximation: Fully self-consistent $GW$ calculations
• Multitier self-consistent $GW$+EDMFT
• On The Relation Between Equation-of-Motion Coupled-Cluster Theory and the GW Approximation
• Low-order Scaling $G_0{W}_0$ by Pair Atomic Density Fitting
• Self-consistent solution of Hedin's equations: semiconductors/insulators
• Ground State Properties of Simple Elements from GW Calculations
• Accurate energy bands calculated by the hybrid quasiparticle self-consistent GW method implemented in the ecalj package
• Ab Initio Full Cell GW+DMFT for Correlated Materials
• QS$G\hat{W}$: Quasiparticle Self consistent $GW$ with ladder diagrams in $W$
• All-electron periodic $G_0{W}_0$ implementation with numerical atomic orbital basis functions: algorithm and benchmarks
• An Optimally-Tuned Starting Point for Single-Shot $GW$ Calculations of Solids
• Exploring the Statically Screened $G3W2$ Correction to the $GW$ Self-Energy: Charged Excitations and Total Energies of Finite Systems
• Lattice polarization effects on the screened Coulomb interaction $W$ of the GW approximation
• Comparing self-consistent GW and vertex corrected G0W0 (G0W0Γ) accuracy for molecular ionization potentials
• Justifying quasiparticle self-consistent schemes via gradient optimization in Luttinger-Ward theory
• A similarity renormalization group approach to Green's function methods
• Full versus quasi-particle self consistency in vertex corrected GW approaches
• Convergence of quasiparticle self-consistent GW calculations of transition metal monoxides
• Broken-symmetry self-consistent GW approach: degree of spin contamination and evaluation of effective exchange couplings in solid antiferromagnets
• Two-component $GW$ calculations: Cubic scaling implementation and comparison of vertex corrected and partially self-consistent $GW$ variants
• Diatomic molecule as a testbed for combining DMFT with electronic structure methods such as $GW$ and DFT
• Gaussian-Based Quasiparticle Self-Consistent $GW$ for Periodic Systems
• Beyond quasi-particle self-consistent $GW$ for molecules with vertex corrections
• A finite electric-field approach to evaluate the vertex correction for the screened Coulomb interaction in the quasiparticle self-consistent GW method
• Many body theory beyond GW : towards a complete description of 2-body correlated propagation
• Low-scaling \textit{GW} calculations of quasi-particle energies for extended systems within the numerical atomic orbital framework