Skip to main content
OSTI.GOVU.S. Department of Energy Office of Scientific and Technical Information
U.S. Department of Energy
Office of Scientific and Technical Information
 

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

Journal Article · · Journal of Physical Chemistry Letters
 [1];  [1];  [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\
+ Show Author Affiliations
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.
Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Complex Materials from First Principles (CCM); Temple Univ., Philadelphia, PA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0012575
OSTI ID:
1566537
Journal Information:
Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 3 Vol. 10; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (39)

Random-phase approximation and its applications in computational chemistry and materials science journal June 2012
30.4-nm He (II) photoelectron spectra of organic molecules journal January 1982
All-electron GW approximation with the mixed basis expansion based on the full-potential LMTO method journal March 2002
A new hybrid exchange–correlation functional using the Coulomb-attenuating method (CAM-B3LYP) journal July 2004
GW 100: Benchmarking G 0 W 0 for Molecular Systems journal November 2015
Quasi-Particle Self-Consistent GW for Molecules journal May 2016
Generalized Optimized Effective Potential for Orbital Functionals and Self-Consistent Calculation of Random Phase Approximations journal September 2017
Challenges for Density Functional Theory journal December 2011
The GW -Method for Quantum Chemistry Applications: Theory and Implementation journal December 2012
Benchmarking the Starting Points of the GW Approximation for Molecules journal December 2012
A comparison of potential molecular wires as components for molecular electronics journal December 2002
Making the random phase approximation to electronic correlation accurate journal October 2009
Hybrid functionals including random phase approximation correlation and second-order screened exchange journal March 2010
Assessment of the Perdew–Burke–Ernzerhof exchange-correlation functional journal March 1999
Toward reliable density functional methods without adjustable parameters: The PBE0 model journal April 1999
Singles correlation energy contributions in solids journal September 2015
The GW method journal March 1998
exciting: a full-potential all-electron package implementing density-functional theory and many-body perturbation theory journal August 2014
Combining GW calculations with exact-exchange density-functional theory: an analysis of valence-band photoemission for compound semiconductors journal January 2005
Inhomogeneous Electron Gas journal November 1964
New Method for Calculating the One-Particle Green's Function with Application to the Electron-Gas Problem journal August 1965
Self-Consistent Equations Including Exchange and Correlation Effects journal November 1965
Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density journal January 1988
Self-consistent GW 0 results for the electron gas: Fixed screened potential W 0 within the random-phase approximation journal September 1996
Fully self-consistent GW self-energy of the electron gas journal January 1998
Self-consistent G W calculations for semiconductors and insulators journal June 2007
Quasiparticle band structure based on a generalized Kohn-Sham scheme journal September 2007
Conserving G W scheme for nonequilibrium quantum transport in molecular contacts journal March 2008
Fully self-consistent GW calculations for molecules journal February 2010
First-principles GW calculations for fullerenes, porphyrins, phtalocyanine, and other molecules of interest for organic photovoltaic applications journal March 2011
First-principles GW calculations for DNA and RNA nucleobases journal March 2011
Unified description of ground and excited states of finite systems: The self-consistent G W approach journal August 2012
Beyond the G W approximation: A second-order screened exchange correction journal August 2015
Accurate all-electron G 0 W 0 quasiparticle energies employing the full-potential augmented plane-wave method journal July 2016
First-Principles Theory of Quasiparticles: Calculation of Band Gaps in Semiconductors and Insulators journal September 1985
Generalized Gradient Approximation Made Simple journal October 1996
All-Electron Self-Consistent G W Approximation: Application to Si, MnO, and NiO journal September 2004
Quasiparticle Self-Consistent G W Theory journal June 2006
Electronic excitations: density-functional versus many-body Green’s-function approaches journal June 2002

Cited By (2)

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 journal July 2019

Similar Records

Approximating Quasiparticle and Excitation Energies from Ground State Generalized Kohn–Sham Calculations
Journal Article · Wed Dec 26 19:00:00 EST 2018 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory · OSTI ID:1566514

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
catalysis (heterogeneous)
electrocatalysis
magnetism and spin physics
materials and chemistry by design
mechanical behavior
solar (photovoltaic)
superconductivity
synthesis (novel materials)
water