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 G_RS 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:

Jin, Ye ^[1]; Su, Neil Qiang  ^[1];

• Search DOE PAGES for author "Su, Neil Qiang"
• Search DOE PAGES for ORCID "0000-0001-7133-2502"

Yang, Weitao  ^[2]

• Search DOE PAGES for author "Yang, Weitao"
• Search DOE PAGES for ORCID "0000-0001-5576-2828"

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+ Show Author Affiliations

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:

Fri Jan 04 00:00:00 EST 2019

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)