BerkeleyGW: A massively parallel computer package for the calculation of the quasiparticle and optical properties of materials and nanostructures

Abstract BerkeleyGW is a massively parallel computational package for electron excited-state properties that is based on the many-body perturbation theory employing the ab initio GW and GW plus Bethe–Salpeter equation methodology. It can be used in conjunction with many density-functional theory codes for ground-state properties, including PARATEC , PARSEC , Quantum ESPRESSO , SIESTA , and Octopus . The package can be used to compute the electronic and optical properties of a wide variety of material systems from bulk semiconductors and metals to nanostructured materials and molecules. The package scales to 10 000s of CPUs and can be used to study systems containing up to 100s of atoms. Program summary Program title: BerkeleyGW Catalogue identifier: AELG_v1_0 Program summary URL: http://cpc.cs.qub.ac.uk/summaries/AELG_v1_0.html Program obtainable from: CPC Program Library, Queenʼs University, Belfast, N. Ireland Licensing provisions: Open source BSD License. See code for licensing details. No. of lines in distributed program, including test data, etc.: 576 540 No. of bytes in distributed program, including test data, etc.: 110 608 809 Distribution format: tar.gz Programming language: Fortran 90, C, C++, Python, Perl, BASH Computer: Linux/UNIX workstations or clusters Operating system: Tested on a variety of Linux distributions in parallel and serial as well as AIX and Mac OSX RAM: (50–2000) MB per CPU (Highly dependent on system size) Classification: 7.2, 7.3, 16.2, 18 External routines: BLAS, LAPACK, FFTW, ScaLAPACK (optional), MPI (optional). All available under open-source licenses. Nature of problem: The excited state properties of materials involve the addition or subtraction of electrons as well as the optical excitations of electron–hole pairs. The excited particles interact strongly with other electrons in a material system. This interaction affects the electronic energies, wavefunctions and lifetimes. It is well known that ground-state theories, such as standard methods based on density-functional theory, fail to correctly capture this physics. Solution method: We construct and solve the Dysonʼs equation for the quasiparticle energies and wavefunctions within the GW approximation for the electron self-energy. We additionally construct and solve the Bethe–Salpeter equation for the correlated electron–hole (exciton) wavefunctions and excitation energies. Restrictions: The material size is limited in practice by the computational resources available. Materials with up to 500 atoms per periodic cell can be studied on large HPCs. Additional comments: The distribution file for this program is approximately 110 Mbytes and therefore is not delivered directly when download or E-mail is requested. Instead a html file giving details of how the program can be obtained is sent. Running time: 1–1000 minutes (depending greatly on system size and processor number).

[1]  S. Louie,et al.  Electron-hole excitations and optical spectra from first principles , 2000 .

[2]  Li Yang,et al.  Excitonic effects on the optical response of graphene and bilayer graphene. , 2009, Physical Review Letters.

[3]  L. Hedin,et al.  Effects of Electron-Electron and Electron-Phonon Interactions on the One-Electron States of Solids , 1969 .

[4]  C. Spataru,et al.  Electron excitations in solids and novel materials , 2004 .

[5]  Takao Kotani,et al.  Quasiparticle self-consistent GW theory. , 2006, Physical review letters.

[6]  Matthew F. Chisholm,et al.  Optical functions of chemical vapor deposited thin‐film silicon determined by spectroscopic ellipsometry , 1993 .

[7]  Jack Deslippe,et al.  Bound excitons in metallic single-walled carbon nanotubes. , 2007, Nano letters.

[8]  Eric L. Shirley,et al.  Optical Absorption of Insulators and the Electron-Hole Interaction: An Ab Initio Calculation , 1998 .

[9]  Alfonso Baldereschi,et al.  Mean-value point and dielectric properties of semiconductors and insulators , 1978 .

[10]  Steven G. Louie,et al.  Conceptual foundations of materials : a standard model for ground- and excited-state properties , 2006 .

[11]  W. Kohn,et al.  Self-Consistent Equations Including Exchange and Correlation Effects , 1965 .

[12]  Eric L. Shirley,et al.  Ab initio calculation of ε 2 ( ω ) including the electron-hole interaction: Application to GaN and CaF 2 , 1999 .

[13]  Steven G. Louie,et al.  Self-consistent pseudopotential method for localized configurations: molecules , 1975 .

[14]  H. Appel,et al.  octopus: a tool for the application of time‐dependent density functional theory , 2006 .

[15]  D. Sánchez-Portal,et al.  The SIESTA method for ab initio order-N materials simulation , 2001, cond-mat/0111138.

[16]  S. Ismail-Beigi.  Truncation of periodic image interactions for confined systems , 2006, cond-mat/0603448.

[17]  Andrzej Fleszar,et al.  Dielectric Response in Semiconductors: Theory and Applications , 1985 .

[18]  Ed Anderson,et al.  LAPACK Users' Guide , 1995 .

[19]  Ariel Biller,et al.  Quasiparticle and optical spectroscopy of the organic semiconductors pentacene and PTCDA from first principles , 2012 .

[20]  N. M. Hugenholtz,et al.  Quantum theory of many-body systems , 1965 .

[21]  Y. Saad,et al.  Finite-difference-pseudopotential method: Electronic structure calculations without a basis. , 1994, Physical review letters.

[22]  Louie,et al.  Electron correlation in semiconductors and insulators: Band gaps and quasiparticle energies. , 1986, Physical review. B, Condensed matter.

[23]  Anton Kokalj,et al.  Computer graphics and graphical user interfaces as tools in simulations of matter at the atomic scale , 2003 .

[24]  F. Aryasetiawan,et al.  The GW method , 1997, cond-mat/9712013.

[25]  Á. Rubio,et al.  octopus: a first-principles tool for excited electron-ion dynamics. , 2003 .

[26]  Steven G. Louie,et al.  Quasiparticle properties of a simple metal at high electron temperatures , 2002 .

[27]  Steven G. Johnson,et al.  The Design and Implementation of FFTW3 , 2005, Proceedings of the IEEE.

[28]  Alexandre M. Zagoskin,et al.  Quantum Theory of Many-Body Systems , 2012 .

[29]  G. Strinati.  Application of the Green’s functions method to the study of the optical properties of semiconductors , 1988 .

[30]  L. Hedin.  NEW METHOD FOR CALCULATING THE ONE-PARTICLE GREEN'S FUNCTION WITH APPLICATION TO THE ELECTRON-GAS PROBLEM , 1965 .

[31]  U. V. Barth,et al.  Fully self-consistent GW self-energy of the electron gas , 1998 .

[32]  Burke,et al.  Generalized Gradient Approximation Made Simple. , 1996, Physical review letters.

[33]  S. Louie,et al.  Quasiparticle energies, excitonic effects and optical absorption spectra of small-diameter single-walled carbon nanotubes , 2004 .

[34]  S. Louie,et al.  Quasiparticle band gap of ZnO: high accuracy from the conventional G⁰W⁰ approach. , 2010, Physical review letters.

[35]  Yasaman Bahri,et al.  Spatial resolution of a type II heterojunction in a single bipolar molecule. , 2009, Nano letters.

[36]  David A. Strubbe,et al.  First-principles prediction of optical second-order harmonic generation in the endohedralN@C60compound , 2011 .

[37]  Stefano de Gironcoli,et al.  QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials , 2009, Journal of physics. Condensed matter : an Institute of Physics journal.

[39]  S. Louie,et al.  Chapter 2 Predicting Materials and Properties: Theory of the Ground and Excited State , 2006 .

[40]  Lucia Reining,et al.  Effect of self-consistency on quasiparticles in solids , 2006 .

[41]  Stefan Albrecht Lucia Reining Rodolfo Del Sole Giovanni Onida.  Ab Initio Calculation of Excitonic Effects in the Optical Spectra of Semiconductors , 1998 .

[42]  Zhang,et al.  Evaluation of quasiparticle energies for semiconductors without inversion symmetry. , 1989, Physical review. B, Condensed matter.

[43]  R. Haydock.  The recursive solution of the Schrödinger equation , 1980 .

[44]  R. Martin,et al.  Electronic Structure: Basic Theory and Practical Methods , 2004 .

[45]  S. Louie,et al.  Excitonic effects and optical spectra of single-walled carbon nanotubes. , 2003, Physical review letters.

[46]  S. Louie,et al.  Renormalization of molecular electronic levels at metal-molecule interfaces. , 2006, Physical Review Letters.

[47]  Matthias Scheffler,et al.  Combining GW calculations with exact-exchange density-functional theory: an analysis of valence-band photoemission for compound semiconductors , 2005, cond-mat/0502404.

[48]  N. Marzari,et al.  Maximally localized Wannier functions for entangled energy bands , 2001, cond-mat/0108084.

[49]  Z. Merali.  Computational science: ...Error , 2010, Nature.

[50]  James R. Chelikowsky,et al.  Real-space pseudopotential method for computing the electronic properties of periodic systems , 2004 .

[51]  Louie,et al.  Ab initio static dielectric matrices from the density-functional approach. I. Formulation and application to semiconductors and insulators. , 1987, Physical review. B, Condensed matter.

[52]  S G Louie,et al.  Coupling of nonlocal potentials to electromagnetic fields. , 2001, Physical review letters.

[53]  N. Marzari,et al.  Maximally localized generalized Wannier functions for composite energy bands , 1997, cond-mat/9707145.

[54]  M. L. Tiago.  Electronic and optical properties of organic crystals, polymers, and semiconductors , 2003 .

[55]  Werner Hanke,et al.  Dielectric theory of elementary excitations in crystals , 1978 .