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

doi:10.1063/1.5126214

This content will become publicly available on December 14, 2020

Title: Improving the efficiency of G ₀ W ₀ calculations with approximate spectral decompositions of dielectric matrices

Abstract

Recently, it was shown that the calculation of quasiparticle energies using the G ₀W ₀ 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 G ₀W ^{0 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:

^[1];

^[2];

^[2]

Univ. of Chicago, IL (United States). Pritzker School of Molecular Engineering
Univ. of Chicago, IL (United States). Pritzker School of Molecular Engineering; Argonne National Lab. (ANL), Lemont, IL (United States)

Publication Date:: 2019-12-14

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: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:10.1063/1.5126214.

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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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Works referenced in this record:

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This content will become publicly available on December 14, 2020

Title: Improving the efficiency of G 0 W 0 calculations with approximate spectral decompositions of dielectric matrices

Abstract

Citation Formats

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

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

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

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

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

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

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

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

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

Random-phase approximation correlation energies from Lanczos chains and an optimal basis set: Theory and applications to the benzene dimer journal, May 2014

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

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

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

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

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

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

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

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

Large Scale GW Calculations journal, May 2015

Title: Improving the efficiency of G ₀ W ₀ calculations with approximate spectral decompositions of dielectric matrices

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

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

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

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

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

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

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

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

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

Random-phase approximation correlation energies from Lanczos chains and an optimal basis set: Theory and applications to the benzene dimer
journal, May 2014

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

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

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

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

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

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

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

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

Large Scale GW Calculations
journal, May 2015