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Title: molgw 1: Many-body perturbation theory software for atoms, molecules, and clusters

Journal Article · · Computer Physics Communications
ORCiD logo [1];  [2];  [3];  [4];  [4];  [5]
  1. Alternative Energies and Atomic Energy Commission (CEA), Gif-sur-Yvette (France). Direction de l'Energie Nucleaire (DEN), Service de Recherches de Metallurgie Physique (SRMP); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Univ. of California, Berkeley, CA (United States). Dept. of Physics
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Univ. of California, Berkeley, CA (United States). Dept. of Physics
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Univ. of California, Berkeley, CA (United States). Dept. of Physics; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Univ. of California, Berkeley, CA (United States). Kavli Energy Nanosciences Inst.
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Computational Research Division
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Univ. of California, Berkeley, CA (United States). Dept. of Physics; Univ. of California, Berkeley, CA (United States). Kavli Energy Nanosciences Inst.
+ Show Author Affiliations

Here, we summarize the MOLGW code that implements density-functional theory and many-body perturbation theory in a Gaussian basis set. The code is dedicated to the calculation of the many-body self-energy within the GW approximation and the solution of the Bethe–Salpeter equation. These two types of calculations allow the user to evaluate physical quantities that can be compared to spectroscopic experiments. Quasiparticle energies, obtained through the calculation of the GW self-energy, can be compared to photoemission or transport experiments, and neutral excitation energies and oscillator strengths, obtained via solution of the Bethe–Salpeter equation, are measurable by optical absorption. The implementation choices outlined here have aimed at the accuracy and robustness of calculated quantities with respect to measurements. Furthermore, the algorithms implemented in MOLGW allow users to consider molecules or clusters containing up to 100 atoms with rather accurate basis sets, and to choose whether or not to apply the resolution-of-the-identity approximation. Finally, we demonstrate the parallelization efficacy of the MOLGW code over several hundreds of processors.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231; 2015-096018
OSTI ID:
1398433
Alternate ID(s):
OSTI ID: 1396452
Journal Information:
Computer Physics Communications, Vol. 208, Issue C; ISSN 0010-4655
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 120 works
Citation information provided by
Web of Science

References (83)

Note on an Approximation Treatment for Many-Electron Systems journal October 1934
New Method for Calculating the One-Particle Green's Function with Application to the Electron-Gas Problem journal August 1965
Dynamical Correlation Effects on the Quasiparticle Bloch States of a Covalent Crystal journal July 1980
First-Principles Theory of Quasiparticles: Calculation of Band Gaps in Semiconductors and Insulators journal September 1985
The GW method journal March 1998
GW quasiparticle calculations in atoms journal June 1993
High Accuracy Many-Body Calculational Approaches for Excitations in Molecules journal January 2001
Variational energy functionals tested on atoms journal May 2004
Optical excitations in organic molecules, clusters, and defects studied by first-principles Green’s function methods journal May 2006
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
An O ( N 3 ) implementation of Hedin's GW approximation for molecules journal August 2011
Ionization energy of atoms obtained from GW self-energy or from random phase approximation total energies journal May 2012
Benchmark of G W methods for azabenzenes journal December 2012
Unified description of ground and excited states of finite systems: The self-consistent G W approach journal August 2012
Bond Breaking and Bond Formation: How Electron Correlation is Captured in Many-Body Perturbation Theory and Density-Functional Theory journal April 2013
Fully self-consistent G W and quasiparticle self-consistent G W for molecules journal April 2014
Molecular Distortions and Chemical Bonding of a Large π -Conjugated Molecule on a Metal Surface journal January 2005
Renormalization of Molecular Electronic Levels at Metal-Molecule Interfaces journal November 2006
Length Dependence of Conductance in Aromatic Single-Molecule Junctions journal November 2009
Transport properties of molecular junctions from many-body perturbation theory journal July 2011
Self-consistent GW calculations of electronic transport in thiol- and amine-linked molecular junctions journal March 2011
ABINIT: First-principles approach to material and nanosystem properties journal December 2009
yambo: An ab initio tool for excited state calculations journal August 2009
SaX: An open source package for electronic-structure and optical-properties calculations in the GW approximation journal August 2009
Implementation and performance of the frequency-dependent G W method within the PAW framework journal July 2006
BerkeleyGW: A massively parallel computer package for the calculation of the quasiparticle and optical properties of materials and nanostructures journal June 2012
GW quasiparticle spectra from occupied states only journal March 2010
Large Scale GW Calculations journal May 2015
Ab initio molecular simulations with numeric atom-centered orbitals journal November 2009
The GW -Method for Quantum Chemistry Applications: Theory and Implementation journal December 2012
A systematic benchmark of the ab initio Bethe-Salpeter equation approach for low-lying optical excitations of small organic molecules journal June 2015
Benchmarking the Starting Points of the GW Approximation for Molecules journal December 2012
Resolution-of-identity approach to Hartree–Fock, hybrid density functionals, RPA, MP2 and GW with numeric atom-centered orbital basis functions journal May 2012
Benchmarking the Bethe–Salpeter Formalism on a Standard Organic Molecular Set journal June 2015
0–0 Energies Using Hybrid Schemes: Benchmarks of TD-DFT, CIS(D), ADC(2), CC2, and BSE/ GW formalisms for 80 Real-Life Compounds journal October 2015
Accurate Ionization Potentials and Electron Affinities of Acceptor Molecules III: A Benchmark of GW Methods journal January 2016
Application of the Green’s functions method to the study of the optical properties of semiconductors journal December 1988
Electronic excitations: density-functional versus many-body Green’s-function approaches journal June 2002
Self-consistent G W calculations for semiconductors and insulators journal June 2007
All-Electron Self-Consistent G W Approximation: Application to Si, MnO, and NiO journal September 2004
Effect of self-consistency on quasiparticles in solids journal July 2006
Fully self-consistent GW calculations for atoms and molecules journal October 2006
Transformation between Cartesian and pure spherical harmonic Gaussians journal April 1995
A new mixing of Hartree–Fock and local density‐functional theories journal January 1993
Toward reliable density functional methods without adjustable parameters: The PBE0 model journal April 1999
Fundamental and excitation gaps in molecules of relevance for organic photovoltaics from an optimally tuned range-separated hybrid functional journal August 2011
Hybrid functionals based on a screened Coulomb potential journal May 2003
Erratum: “Hybrid functionals based on a screened Coulomb potential” [J. Chem. Phys. 118, 8207 (2003)] journal June 2006
Efficient recursive computation of molecular integrals over Cartesian Gaussian functions journal April 1986
A quantitative study of the scaling properties of the Hartree–Fock method journal June 1995
Kohn—Sham density-functional theory within a finite basis set journal November 1992
Libxc: A library of exchange and correlation functionals for density functional theory journal October 2012
A multicenter numerical integration scheme for polyatomic molecules journal February 1988
Achieving linear scaling in exchange-correlation density functional quadratures journal July 1996
Improved radial grids for quadrature in molecular density‐functional calculations journal June 1996
Convergence acceleration of iterative sequences. the case of scf iteration journal July 1980
ImprovedSCF convergence acceleration journal January 1982
Auxiliary basis sets to approximate Coulomb potentials journal June 1995
Auxiliary basis sets for main row atoms and transition metals and their use to approximate Coulomb potentials
  • Eichkorn, Karin; Weigend, Florian; Treutler, Oliver
  • Theoretical Chemistry Accounts: Theory, Computation, and Modeling (Theoretica Chimica Acta), Vol. 97, Issue 1-4 https://doi.org/10.1007/s002140050244
journal October 1997
A fully direct RI-HF algorithm: Implementation, optimised auxiliary basis sets, demonstration of accuracy and efficiency journal August 2002
Time-Dependent Hartree—Fock Theory for Molecules journal July 1964
Total Energies from GW Calculations journal July 1999
Variational energy functionals of the Green function and of the density tested on molecules journal January 2006
Perturbation Theory for an Infinite Medium of Fermions. II journal February 1961
Successful Test of a Seamless van der Waals Density Functional journal March 1999
Molecular tests of the random phase approximation to the exchange-correlation energy functional journal October 2001
Developing the random phase approximation into a practical post-Kohn–Sham correlation model journal September 2008
Electron correlation in semiconductors and insulators: Band gaps and quasiparticle energies journal October 1986
Local-field and excitonic effects in the optical spectrum of a covalent crystal journal November 1975
Ab Initio Calculation of Excitonic Effects in the Optical Spectra of Semiconductors journal May 1998
Ab Initio Inclusion of Electron-Hole Attraction: Application to X-Ray Absorption and Resonant Inelastic X-Ray Scattering journal January 1998
Electron-Hole Excitations in Semiconductors and Insulators journal September 1998
GW and Bethe-Salpeter study of small water clusters journal January 2016
The role of databases in support of computational chemistry calculations journal October 1996
Basis Set Exchange:  A Community Database for Computational Sciences journal March 2007
NWChem: A comprehensive and scalable open-source solution for large scale molecular simulations journal September 2010
Efficient use of the correlation consistent basis sets in resolution of the identity MP2 calculations journal February 2002
Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen journal January 1989
Electron affinities of the first‐row atoms revisited. Systematic basis sets and wave functions journal May 1992
Accurate G W self-energies in a plane-wave basis using only a few empty states: Towards large systems journal August 2008
Coulomb-hole summations and energies for G W calculations with limited number of empty orbitals: A modified static remainder approach journal April 2013
Structure preserving parallel algorithms for solving the Bethe–Salpeter eigenvalue problem journal January 2016

Cited By (14)

Practical GW scheme for electronic structure of 3 d -transition-metal monoxide anions: ScO−, TiO−, CuO−, and ZnO− journal October 2019
Separable resolution-of-the-identity with all-electron Gaussian bases: Application to cubic-scaling RPA journal May 2019
Ab initio modelling of local interfaces in doped organic semiconductors journal January 2020
Propagation of maximally localized Wannier functions in real-time TDDFT journal May 2019
All-electron ab initio Bethe-Salpeter equation approach to neutral excitations in molecules with numeric atom-centered orbitals journal January 2020
Screening mixing GW/Bethe–Salpeter approach for triplet states of organic molecules journal September 2018
The GW Compendium: A Practical Guide to Theoretical Photoemission Spectroscopy journal July 2019
Modeling Excited States of Confined Systems book January 2018
Modeling Excited States of Confined Systems book January 2020
Separable Resolution-of-the-Identity with All-Electron Gaussian Bases: Application to Cubic-scaling RPA text January 2019
Many-body perturbation theory calculations using the yambo code text January 2019
Propagation of maximally localized Wannier functions in real-time TDDFT text January 2019
Interplay between Intra- and Intermolecular Charge Transfer in the Optical Excitations of J-Aggregates journal February 2019
Questaal: a package of electronic structure methods based on the linear muffin-tin orbital technique text January 2019

Linked Research (2)

Figures / Tables (10)

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Table 1(p. 12)table Table 1
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Figure 7(p. 14)figure Figure 7
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Figure 9(p. 16)figure Figure 9

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Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
97 MATHEMATICS AND COMPUTING
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS
Electronic structure of molecules
Many-body perturbation theory
GW approximation
Bethe–Salpeter equation