Renormalized Singles with Correlation in $GW$ Green's Function Theory for Accurate Quasiparticle Energies

Abstract

We apply the renormalized singles with correlation (RSc) Green's function in the $GW$ approximation to calculate accurate quasiparticle (QP) energies and orbitals. The RSc Green's function includes all orders of singles contributions from the associated density functional approximation (DFA) and treats higher order contributions in a perturbative manner. The $G_{\text{RSc}}{W}_{\text{RSc}}$ method uses the RSc Green's function as the new starting point and calculates the screened interaction with the RSc Green's function. The $G_{\text{RSc}}{W}_0$ methods fixes the screened interaction at the DFA level. For the calculations of ionization potentials in the GW100 set, $G_{\text{RSc}}{W}_{\text{RSc}}$ significantly reduces the dependence on the starting point of DFAs used and provides accurate results with the mean absolute error (MAE) of $0.34$ eV comparable to ev$GW$. For the calculations of core-level binding energies in the CORE65 set, $G_{\text{RSc}}{W}_{\text{RSc}}$ slightly overestimates the results because of underscreening, but $G_{\text{RSc}}{W}_0$ with GGA functionals provides the optimal accuracy of $0.40$ eV MAE comparable to ev$G{W}_0$. We also show that $G_{\text{RSc}}{W}_{\text{RSc}}$ predicts accurate dipole moments of small molecules. These two methods, $G_{\text{RSc}}{W}_{\text{RSc}}$ and $G_{\text{RSc}}{W}_0$, are computationally much favorable than any flavor of self-consistent $GW$ methods. Thus, the RSc approach is promising for making $GW$ and other Green's function methods efficient and robust.

References in corpus (38)

• Localization and delocalization errors in density functional theory and implications for band-gap prediction
• 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
• Fractional charge perspective on the band-gap in density-functional theory
• All-electron self-consistent GW approximation: Application to Si, MnO, and NiO
• Quasiparticle band structure based on a generalized Kohn-Sham scheme
• Quasiparticle self-consistent $GW$ method; a basis for the independent-particle approximation
• The GW compendium: A practical guide to theoretical photoemission spectroscopy
• Quasiparticle spectra from a non-empirical optimally-tuned range-separated hybrid density functional
• Fully selfconsistent GW calculations for molecules
• The discontinuous nature of the exchange-correlation functional -- critical for strongly correlated systems
• Beyond the Random Phase Approximation for the Electron Correlation Energy: The Importance of Single Excitations
• 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?
• Levels of self-consistency in the GW approximation
• Self-consistent GW: All-electron implementation with localized basis functions
• Assessment of correlation energies based on the random-phase approximation
• Localized Orbital Scaling Correction for Systematic Elimination of Delocalization Error in Density Functional Approximations
• Quasi-Particle Self-Consistent $GW$ for Molecules
• Towards GW Calculations on Thousands of Atoms
• Exchange and Correlation in Open Systems of Fluctuating Electron Number
• Benchmark of GW approaches for the GW100 testset
• Accurate absolute and relative core-level binding energies from $GW$
• Fully self-consistent $GW$ and quasi-particle self-consistent $GW$ for molecules
• Beyond the GW approximation: combining correlation channels
• Cubic-scaling all-electron GW calculations with a separable density-fitting space-time approach
• All-electron GW calculation for molecules: Ionization energy and electron affinity of conjugated molecules
• All-electron Gaussian-based $G_0{W}_0$ for Valence and Core Excitation Energies of Periodic Systems
• Ab Initio Full Cell GW+DMFT for Correlated Materials
• All-electron periodic $G_0{W}_0$ implementation with numerical atomic orbital basis functions: algorithm and benchmarks
• Approximating Quasiparticle and Excitation Energies from Ground State Generalized Kohn-Sham Calculations
• Renormalized Singles Green's Function in the T-Matrix Approximation for Accurate Quasiparticle Energy Calculation
• Piecewise linearity in the $GW$ approximation for accurate quasiparticle energy predictions
• On the basis set selection for molecular core-level $GW$ calculations
• Unphysical Discontinuities, Intruder States and Regularization in $GW$ Methods
• Scrutinizing $GW$-based methods using the Hubbard dimer
• Multireference Density Functional Theory for Describing Ground and Excited States with Renormalized Singles
• Combining Localized Orbital Scaling Correction and Bethe-Salpeter Equation for Accurate Excitation Energies

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