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Title: Renormalized Singles Green’s Function for Quasi-Particle Calculations beyond the G0W0 Approximation

Abstract

Quasi-particle energies and band gaps in particular are critical for investigating novel materials. Commonly used density functional approximations (DFAs) systematically underestimate band gaps, and GW approximation is the established method of choice for good accuracy and reliability. However, G0W0 has some undesired dependence on the DFA, while self-consistent GW (scGW) is expensive and not consistent in accuracy improvement. Here a simple and efficient GRS W0 approach has been developed: a subspace diagonalization of the Hartree-Fock (HF) Hamiltonian with the DFA density matrix provides the new reference Green's function GRS that incorporates the effect of all single excitation contributions to the self-energy, thereby essentially eliminating the starting-point dependence. Calculations for molecules and large band gap solids demonstrate the significant improvement over G0W0 and greatly reduced dependence on the initial DFA. GRS W0 approach also improve results for other bulks over G0W0 but to a lesser extent, which could be due to the limitations in current implementation for bulks. The results demonstrate that to achieve good accuracy, it is not necessary to use hybrid DFA, which is expensive for bulks. Lastly, this work should be greatly significant in making GW a more robust approach.

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [2]
  1. Duke Univ., Durham, NC (United States)
  2. Duke Univ., Durham, NC (United States); South China Normal University, Guangzhou (China). Key Lab. of Theoretical Chemistry of Environment\
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Complex Materials from First Principles (CCM); Temple Univ., Philadelphia, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1566537
Grant/Contract Number:  
SC0012575
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 10; Journal Issue: 3; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (heterogeneous); electrocatalysis; solar (photovoltaic); mechanical behavior; superconductivity; magnetism and spin physics; water; materials and chemistry by design; synthesis (novel materials)

Citation Formats

Jin, Ye, Su, Neil Qiang, and Yang, Weitao. Renormalized Singles Green’s Function for Quasi-Particle Calculations beyond the G0W0 Approximation. United States: N. p., 2019. Web. https://doi.org/10.1021/acs.jpclett.8b03337.
Jin, Ye, Su, Neil Qiang, & Yang, Weitao. Renormalized Singles Green’s Function for Quasi-Particle Calculations beyond the G0W0 Approximation. United States. https://doi.org/10.1021/acs.jpclett.8b03337
Jin, Ye, Su, Neil Qiang, and Yang, Weitao. Fri . "Renormalized Singles Green’s Function for Quasi-Particle Calculations beyond the G0W0 Approximation". United States. https://doi.org/10.1021/acs.jpclett.8b03337. https://www.osti.gov/servlets/purl/1566537.
@article{osti_1566537,
title = {Renormalized Singles Green’s Function for Quasi-Particle Calculations beyond the G0W0 Approximation},
author = {Jin, Ye and Su, Neil Qiang and Yang, Weitao},
abstractNote = {Quasi-particle energies and band gaps in particular are critical for investigating novel materials. Commonly used density functional approximations (DFAs) systematically underestimate band gaps, and GW approximation is the established method of choice for good accuracy and reliability. However, G0W0 has some undesired dependence on the DFA, while self-consistent GW (scGW) is expensive and not consistent in accuracy improvement. Here a simple and efficient GRS W0 approach has been developed: a subspace diagonalization of the Hartree-Fock (HF) Hamiltonian with the DFA density matrix provides the new reference Green's function GRS that incorporates the effect of all single excitation contributions to the self-energy, thereby essentially eliminating the starting-point dependence. Calculations for molecules and large band gap solids demonstrate the significant improvement over G0W0 and greatly reduced dependence on the initial DFA. GRS W0 approach also improve results for other bulks over G0W0 but to a lesser extent, which could be due to the limitations in current implementation for bulks. The results demonstrate that to achieve good accuracy, it is not necessary to use hybrid DFA, which is expensive for bulks. Lastly, this work should be greatly significant in making GW a more robust approach.},
doi = {10.1021/acs.jpclett.8b03337},
journal = {Journal of Physical Chemistry Letters},
number = 3,
volume = 10,
place = {United States},
year = {2019},
month = {1}
}

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    Works referencing / citing this record:

    Quantum embedding theory in the screened Coulomb interaction: Combining configuration interaction with G W / BSE
    journal, July 2019


    The GW Compendium: A Practical Guide to Theoretical Photoemission Spectroscopy
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