First-principles GW calculations for fullerenes, porphyrins, phtalocyanine, and other molecules of interest for organic photovoltaic applications

Abstract

We evaluate the performances of ab initio GW calculations for the ionization energies and HOMO-LUMO gaps of thirteen gas phase molecules of interest for organic electronic and photovoltaic applications, including the C60 fullerene, pentacene, free-base porphyrins and phtalocyanine, PTCDA, and standard monomers such as thiophene, fluorene, benzothiazole or thiadiazole. Standard G0W0 calculations, that is starting from eigenstates obtained with local or semilocal functionals, significantly improve the ionization energy and band gap as compared to density functional theory Kohn-Sham results, but the calculated quasiparticle values remain too small as a result of overscreening. Starting from Hartree-Fock-like eigenvalues provides much better results and is equivalent to performing self-consistency on the eigenvalues, with a resulting accuracy of 2~4% as compared to experiment. Our calculations are based on an efficient gaussian-basis implementation of GW with explicit treatment of the dynamical screening through contour deformation techniques.

arXiv comment10 pages, 3 figures

References in corpus (10)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• The SIESTA method for ab initio order-N materials simulation
• Efficient index handling of multidimensional periodic boundary conditions
• Yambo: an \textit{ab initio} tool for excited state calculations
• Fully selfconsistent GW calculations for molecules
• GW method with the self-consistent Sternheimer equation
• Neutral and charged excitations in carbon fullerenes from first-principles many-body theories
• Quasiparticle energies for large molecules: a tight-binding GW approach
• Benchmarking GW against exact diagonalization for semi-empirical models
• On the Kohn--Sham density response in a localized basis set

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