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Title: Improving the efficiency of G0W0 calculations with approximate spectral decompositions of dielectric matrices

Abstract

Recently, it was shown that the calculation of quasiparticle energies using the G0W0 approximation can be performed without computing explicitly any virtual electronic states, by expanding the Green function and screened Coulomb interaction in terms of the eigenstates of the static dielectric matrix. Avoiding the evaluation of virtual electronic states leads to improved efficiency and ease of convergence of G0W0 calculations. Here, we propose a further improvement of the efficiency of these calculations, based on an approximation of density-density response functions of molecules and solids. The approximation relies on the calculation of a subset of eigenvectors of the dielectric matrix using the kinetic operator instead of the full Hamiltonian, and it does not lead to any substantial loss of accuracy for the quasiparticle energies. The computational savings introduced by this approximation depend on the system, and they become more substantial as the number of electrons increases.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]
+ Show Author Affiliations
  1. Univ. of Chicago, IL (United States). Pritzker School of Molecular Engineering
  2. Univ. of Chicago, IL (United States). Pritzker School of Molecular Engineering; Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1595951
Alternate Identifier(s):
OSTI ID: 1577886
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 22; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Yang, Han, Govoni, Marco, and Galli, Giulia. Improving the efficiency of G0W0 calculations with approximate spectral decompositions of dielectric matrices. United States: N. p., 2019. Web. doi:10.1063/1.5126214.
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Yang, Han, Govoni, Marco, & Galli, Giulia. Improving the efficiency of G0W0 calculations with approximate spectral decompositions of dielectric matrices. United States. doi:https://doi.org/10.1063/1.5126214
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Yang, Han, Govoni, Marco, and Galli, Giulia. Sat . "Improving the efficiency of G0W0 calculations with approximate spectral decompositions of dielectric matrices". United States. doi:https://doi.org/10.1063/1.5126214. https://www.osti.gov/servlets/purl/1595951.
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@article{osti_1595951,
title = {Improving the efficiency of G0W0 calculations with approximate spectral decompositions of dielectric matrices},
author = {Yang, Han and Govoni, Marco and Galli, Giulia},
abstractNote = {Recently, it was shown that the calculation of quasiparticle energies using the G0W0 approximation can be performed without computing explicitly any virtual electronic states, by expanding the Green function and screened Coulomb interaction in terms of the eigenstates of the static dielectric matrix. Avoiding the evaluation of virtual electronic states leads to improved efficiency and ease of convergence of G0W0 calculations. Here, we propose a further improvement of the efficiency of these calculations, based on an approximation of density-density response functions of molecules and solids. The approximation relies on the calculation of a subset of eigenvectors of the dielectric matrix using the kinetic operator instead of the full Hamiltonian, and it does not lead to any substantial loss of accuracy for the quasiparticle energies. The computational savings introduced by this approximation depend on the system, and they become more substantial as the number of electrons increases.},
doi = {10.1063/1.5126214},
journal = {Journal of Chemical Physics},
number = 22,
volume = 151,
place = {United States},
year = {2019},
month = {12}
}
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DOI:  https://doi.org/10.1063/1.5126214
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Works referenced in this record:

Electron correlation and the band gap in ionic crystals
journal, November 1985

Subnitride and valence band offset at Si3N4∕Si interface formed using nitrogen-hydrogen radicals
journal, March 2007

  • Higuchi, Masaaki; Sugawa, Shigetoshi; Ikenaga, Eiji
  • Applied Physics Letters, Vol. 90, Issue 12
  • DOI: 10.1063/1.2715037

Generalization of Dielectric-Dependent Hybrid Functionals to Finite Systems
journal, October 2016

Theoretical study of band offsets at semiconductor interfaces
journal, May 1987

Valence and core photoelectron spectroscopy of C60, buckminsterfullerene
journal, January 1991

  • Lichtenberger, Dennis L.; Nebesny, Kenneth W.; Ray, Charles D.
  • Chemical Physics Letters, Vol. 176, Issue 2
  • DOI: 10.1016/0009-2614(91)90155-3

A Finite-Field Approach for GW Calculations beyond the Random Phase Approximation
journal, November 2018

  • Ma, He; Govoni, Marco; Gygi, Francois
  • Journal of Chemical Theory and Computation, Vol. 15, Issue 1
  • DOI: 10.1021/acs.jctc.8b00864

Ab initio Calculation of van der Waals Bonded Molecular Crystals
journal, May 2009

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009

  • Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
  • Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
  • DOI: 10.1088/0953-8984/21/39/395502

Speeding up GW Calculations to Meet the Challenge of Large Scale Quasiparticle Predictions
journal, November 2016

  • Gao, Weiwei; Xia, Weiyi; Gao, Xiang
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep36849

Simple Approximate Physical Orbitals for G W Quasiparticle Calculations
journal, October 2011

Electron self-energy calculation using a general multi-pole approximation
journal, April 2003

  • Soininen, J. A.; Rehr, J. J.; Shirley, Eric L.
  • Journal of Physics: Condensed Matter, Vol. 15, Issue 17
  • DOI: 10.1088/0953-8984/15/17/312

Phonons and related crystal properties from density-functional perturbation theory
journal, July 2001

  • Baroni, Stefano; de Gironcoli, Stefano; Dal Corso, Andrea
  • Reviews of Modern Physics, Vol. 73, Issue 2
  • DOI: 10.1103/revmodphys.73.515

Improving accuracy and efficiency of calculations of photoemission spectra within the many-body perturbation theory
journal, February 2012

First-principles electrostatic potentials for reliable alignment at interfaces and defects
journal, March 2017

  • Sundararaman, Ravishankar; Ping, Yuan
  • The Journal of Chemical Physics, Vol. 146, Issue 10
  • DOI: 10.1063/1.4978238

Electronic Structure
book, January 2004

Dielectric Properties of Ice and Liquid Water from First-Principles Calculations
journal, April 2008

Dynamical aspects of correlation corrections in a covalent crystal
journal, February 1982

First-Principles Theory of Quasiparticles: Calculation of Band Gaps in Semiconductors and Insulators
journal, September 1985

Optical properties of silicon nitride films deposited by hot filament chemical vapor deposition
journal, June 1995

  • Deshpande, Sadanand V.; Gulari, Erdogan; Brown, Steven W.
  • Journal of Applied Physics, Vol. 77, Issue 12
  • DOI: 10.1063/1.359062

Electron correlation in semiconductors and insulators: Band gaps and quasiparticle energies
journal, October 1986

Geometric and electronic structures of Si O 2 / Si ( 001 ) interfaces
journal, March 2001

Inhomogeneous Electron Gas
journal, November 1964

Quantum Theory of the Dielectric Constant in Real Solids
journal, April 1962

Band offsets and dielectric properties of the amorphous Si 3 N 4 /Si(100) interface: A first-principles study
journal, June 2013

  • Anh Pham, T.; Li, Tianshu; Nguyen, Huy-Viet
  • Applied Physics Letters, Vol. 102, Issue 24
  • DOI: 10.1063/1.4811481

GW 100: A Plane Wave Perspective for Small Molecules
journal, January 2017

  • Maggio, Emanuele; Liu, Peitao; van Setten, Michiel J.
  • Journal of Chemical Theory and Computation, Vol. 13, Issue 2
  • DOI: 10.1021/acs.jctc.6b01150

GW 100: Benchmarking G 0 W 0 for Molecular Systems
journal, November 2015

  • van Setten, Michiel J.; Caruso, Fabio; Sharifzadeh, Sahar
  • Journal of Chemical Theory and Computation, Vol. 11, Issue 12
  • DOI: 10.1021/acs.jctc.5b00453

Dynamical Correlation Effects on the Quasiparticle Bloch States of a Covalent Crystal
journal, July 1980

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/physrevlett.77.3865

Valence band offset at silicon/silicon nitride and silicon nitride/silicon oxide interfaces
journal, August 2003

G W calculations using the spectral decomposition of the dielectric matrix: Verification, validation, and comparison of methods
journal, April 2013

GW100: Comparison of Methods and Accuracy of Results Obtained with the WEST Code
journal, February 2018

  • Govoni, Marco; Galli, Giulia
  • Journal of Chemical Theory and Computation, Vol. 14, Issue 4
  • DOI: 10.1021/acs.jctc.7b00952

Optical properties, band gap, and surface roughness of Si3N4
journal, February 1977

Optimized norm-conserving Vanderbilt pseudopotentials
journal, August 2013

Dielectric Constant with Local Field Effects Included
journal, January 1963

Iterative calculations of dielectric eigenvalue spectra
journal, June 2009

Efficient iterative method for calculations of dielectric matrices
journal, September 2008

Inhomogeneous Electron Gas
journal, March 1973

Electronic Polarizabilities of Ions from the Hartree-Fock Wave Functions
journal, November 1954

Band offsets for ultrathin SiO[sub 2] and Si[sub 3]N[sub 4] films on Si(111) and Si(100) from photoemission spectroscopy
journal, January 1999

  • Keister, J. W.; Rowe, J. E.; Kolodziej, J. J.
  • Journal of Vacuum Science & Technology B: Microelectronics and Nanometer Structures, Vol. 17, Issue 4
  • DOI: 10.1116/1.590834

Electronic excitations: density-functional versus many-body Green’s-function approaches
journal, June 2002

The GW Compendium: A Practical Guide to Theoretical Photoemission Spectroscopy
journal, July 2019

Optimization algorithm for the generation of ONCV pseudopotentials
journal, November 2015

Implementation and Validation of Fully Relativistic GW Calculations: Spin–Orbit Coupling in Molecules, Nanocrystals, and Solids
journal, July 2016

  • Scherpelz, Peter; Govoni, Marco; Hamada, Ikutaro
  • Journal of Chemical Theory and Computation, Vol. 12, Issue 8
  • DOI: 10.1021/acs.jctc.6b00114

Photoemission of Electrons and Holes into Silicon Nitride
journal, October 1968

Assessment of Gaussian-2 and density functional theories for the computation of ionization potentials and electron affinities
journal, July 1998

  • Curtiss, Larry A.; Redfern, Paul C.; Raghavachari, Krishnan
  • The Journal of Chemical Physics, Vol. 109, Issue 1
  • DOI: 10.1063/1.476538

Accurate G W self-energies in a plane-wave basis using only a few empty states: Towards large systems
journal, August 2008

Advanced capabilities for materials modelling with Quantum ESPRESSO
journal, October 2017

  • Giannozzi, P.; Andreussi, O.; Brumme, T.
  • Journal of Physics: Condensed Matter, Vol. 29, Issue 46
  • DOI: 10.1088/1361-648x/aa8f79

Large Scale GW Calculations
journal, May 2015

  • Govoni, Marco; Galli, Giulia
  • Journal of Chemical Theory and Computation, Vol. 11, Issue 6
  • DOI: 10.1021/ct500958p

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965

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