The LDA-1/2 Method Applied to Atoms and Molecules

Pelá, Ronaldo Rodrigues; Guļāns, Andris; Draxl, Claudia

doi:10.1021/acs.jctc.8b00518

Cited by 8 publications

(8 citation statements)

References 37 publications

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“…This set came into existence first in a comparison between only three codes ( van Setten et al, 2015 ). In the meantime the developers of many other codes have used the set to test and benchmark their implementations, both for GW and other computational approaches aiming at the calculation of ionization energies and electron affinities ( Caruso et al, 2016 ; Vlček et al, 2017a ; Maggio et al, 2017 ; Wilhelm and Hutter, 2017 ; Govoni and Galli, 2018 ; Rodrigues Pela et al, 2018 ; Colonna et al, 2019 ; Gao and Chelikowsky, 2019 ; Brémond et al, 2020 ; Förster and Visscher, 2020 ; Gao and Chelikowsky, 2020 ; Bintrim and Berkelbach, 2021 ; Duchemin and Blase, 2021 ; Förster and Visscher, 2021 ; Wilhelm et al, 2021 ). At present over a hundred data sets have appeared for the GW100 set.…”

Section: Ccsd(t) Ionization Potentials For Gw100mentioning

confidence: 99%

The GW Miracle in Many-Body Perturbation Theory for the Ionization Potential of Molecules

2021

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We use the GW100 benchmark set to systematically judge the quality of several perturbation theories against high-level quantum chemistry methods. First of all, we revisit the reference CCSD(T) ionization potentials for this popular benchmark set and establish a revised set of CCSD(T) results. Then, for all of these 100 molecules, we calculate the HOMO energy within second and third-order perturbation theory (PT2 and PT3), and, GW as post-Hartree-Fock methods. We found GW to be the most accurate of these three approximations for the ionization potential, by far. Going beyond GW by adding more diagrams is a tedious and dangerous activity: We tried to complement GW with second-order exchange (SOX), with second-order screened exchange (SOSEX), with interacting electron-hole pairs (WTDHF), and with a GW density-matrix (γGW). Only the γGW result has a positive impact. Finally using an improved hybrid functional for the non-interacting Green’s function, considering it as a cheap way to approximate self-consistency, the accuracy of the simplest GW approximation improves even more. We conclude that GW is a miracle: Its subtle balance makes GW both accurate and fast.

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Section: Ccsd(t) Ionization Potentials For Gw100mentioning

confidence: 99%

The GW Miracle in Many-Body Perturbation Theory for the Ionization Potential of Molecules

2021

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“…30 We also mention that the method has recently been applied successfully for the calculation of the ionization potential of atoms and molecules. 40 However, the limitations of the method have not been given much consideration until recently. 41 These limitations stem from the fact that the correction applied in DFT-1/2 has an atomic origin.…”

Section: Introductionmentioning

confidence: 99%

Limitations of the DFT–1/2 method for covalent semiconductors and transition-metal oxides

2019

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The DFT-1/2 method in density functional theory [L. G. Ferreira et al., Phys. Rev. B 78, 125116 (2008)] aims to provide accurate band gaps at the computational cost of semilocal calculations. The method has shown promise in a large number of cases, however some of its limitations or ambiguities on how to apply it to covalent semiconductors have been pointed out recently [K.-H. Xue et al., Comput. Mater. Science 153, 493 (2018)]. In this work, we investigate in detail some of the problems of the DFT-1/2 method with a focus on two classes of materials: covalently bonded semiconductors and transition-metal oxides. We argue for caution in the application of DFT-1/2 to these materials, and the condition to get an improved band gap is a spatial separation of the orbitals at the valence band maximum and conduction band minimum.

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“…We employed the DFT-1/2 quasiparticle correction developed by Ferreira, Marques, and Teles, 34 which has been widely applied in energy gap predictions for two-dimensional (2D)/three-dimensional (3D) systems 35−38 through codes such as WIEN2K, 34,34 VASP, 37−39 and EXCITING. 40 The DFT-1/2 method was already applied successfully in pure MHP. 39 In the study presented here, we introduce a general procedure for MHP mixtures, or alloys, which also can be applied to 2D MHP, such as Ruddlesden−Popper.…”

mentioning

confidence: 99%

Relativistic DFT-1/2 Calculations Combined with a Statistical Approach for Electronic and Optical Properties of Mixed Metal Hybrid Perovskites

Guedes-Sobrinho

Guilhon

Marques

et al. 2019

J. Phys. Chem. Lett.

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We overcome the great theoretical computational challenge of mixed perovskites, providing a rigorous and efficient model by including quasiparticle, spin−orbit coupling, and disorder effects. As a benchmark, we consider the mixed MAPb 1−x Sn x I 3 perovskites. The calculations are based on the generalized quasichemical approach and the DFT-1/2 approximated quasiparticle correction. Both cubic and tetragonal structures are investigated. By mapping the entire range of compositions, we correctly describe the bowing-like behavior for the energy gaps with 1.24 eV as the minimum value at x = 0.70, in very good agreement with the experimental data. Furthermore, while the tetragonal alloy reaches the maximum absorbance with a limit for the red shift at x = 1.0, the cubic alloy sets a maximum absorbance/red shift for the optimal composition at x = 0.70.

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The LDA-1/2 Method Applied to Atoms and Molecules

Cited by 8 publications

References 37 publications

The GW Miracle in Many-Body Perturbation Theory for the Ionization Potential of Molecules

The GW Miracle in Many-Body Perturbation Theory for the Ionization Potential of Molecules

Limitations of the DFT–1/2 method for covalent semiconductors and transition-metal oxides

Relativistic DFT-1/2 Calculations Combined with a Statistical Approach for Electronic and Optical Properties of Mixed Metal Hybrid Perovskites

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