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Comparing Self-Consistent <i>GW</i> and Vertex-Corrected <i>G</i><sub>0</sub><i>W</i><sub>0</sub> (<i>G</i><sub>0</sub><i>W</i><sub>0</sub>Γ) Accuracy for Molecular Ionization Potentials

Ming Wen, Vibin Abraham, Gaurav Harsha, Avijit Shee, K. Birgitta Whaley, Dominika Zgid

2024Journal of Chemical Theory and Computation27 citationsDOI

Abstract

We test the performance of self-consistent GW and several representative implementations of vertex-corrected G 0 W 0 ( G 0 W 0 Γ). These approaches are tested on benchmark data sets covering full valence spectra (first ionization potentials and some inner valence shell excitations). For small molecules, when comparing against state-of-the-art wave function techniques, our results show that full self-consistency in the GW scheme either systematically outperforms vertex-corrected G 0 W 0 or gives results of at least comparative quality. Moreover, G 0 W 0 Γ results in additional computational cost when compared to G 0 W 0 or self-consistent GW . The dependency of G 0 W 0 Γ on the starting mean-field solution is frequently more dominant than the magnitude of the vertex correction itself. Consequently, for molecular systems, self-consistent GW performed on the imaginary axis (and then followed by modern analytical continuation techniques) offers a more reliable approach to make predictions of ionization potentials.

Topics & Concepts

PhysicsVertex (graph theory)CombinatoricsMathematicsGraphMass Spectrometry Techniques and ApplicationsPesticide Residue Analysis and SafetyChemical Thermodynamics and Molecular Structure
Comparing Self-Consistent <i>GW</i> and Vertex-Corrected <i>G</i><sub>0</sub><i>W</i><sub>0</sub> (<i>G</i><sub>0</sub><i>W</i><sub>0</sub>Γ) Accuracy for Molecular Ionization Potentials | Litcius