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Electron–phonon coupling and charge-transfer excitations in organic systems from many-body perturbation theory

The Fiesta code, an efficient Gaussian-basis implementation of the GW and Bethe–Salpeter formalisms

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Abstract

We review in this article recent developments within the framework of ab initio many-body perturbation theory aiming at providing an accurate description of the electronic and excitonic properties of π-conjugated organic systems currently used in organic photovoltaic cells. In particular, techniques such as the GW and Bethe–Salpeter formalisms are being benchmarked for acenes, fullerenes, porphyrins, phthalocyanines, and other molecules of interest for solar energy applications. It is shown that not only the electronic properties, but also the electron–phonon coupling matrix elements, and the charge-transfer excitations in donor/acceptor complexes, are accurately described. The present calculations on molecules containing up to a hundred atoms are based on a recently developed Gaussian auxiliary basis implementation of the GW and Bethe–Salpeter formalism, including full dynamics with contour-deformation techniques, as implemented in the Fiesta code.

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Notes

  1. This code originates in a previous implementation of TDDFT using the strictly-localized atomic-like orbital basis implemented in the DFT Siesta [55] package, see [56].

  2. In the case of acenes, see: assessment of density-functionalmodels for organic molecular semiconductors: the role of Hartree–Fock exchange in charge-transfer processes, see [75].

  3. The equivalence between the approach based on differencesof total energies, and the one involving individual electron–phonon matrix elements, (compare, e.g., formulas (1) and (4) in Ref. [77]) has been validated numerically for many systems within DFT (see, e.g., in the case of the acenes the results of Refs. [77] and [78]), even though formally the only existing demonstrations assume the coupling between vibrational modes and free electrons at the Fermi level within the so-called independent boson model [79], one of the few exactly solvable many-body problems.

  4. For a review, see [84].

  5. Very similar results are obtained at the PBE level, see Ref. [84].

  6. The lowest 20 % percentage of exact exchange corresponds to the well-known B3LYP functional, see Ref. [91]

  7. An interesting observation is that a non-self-consistent G 0 W 0 calculation starting from LDA eigenstates leads to a coupling constant which is still significantly larger than the DFT–LDA value, but smaller than the GW psc one, and very similar to that of the hybrid B3LYP functional. As emphasized in the introductory section, single-shot G 0 W 0 calculations result in too small HOMO–LUMO gaps, inducing overscreening expected to soften the variations of the ionic and electronic potential seen by the electrons upon lattice distortion, see data in Ref. [51].

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Acknowledgements

Computing time has been provided by the local CIMENT and national IDRIS supercomputing (Project no. 100063) centers in Grenoble and Orsay, respectively. The authors acknowledge Dr. Laflamme Janssen, Pr. Michel Côté, and Pr. Erich Runge, with whom parts of the work presented in this review were achieved, and Pr. Mark Casida for useful discussions.

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Authors and Affiliations

  1. Institut Néel, CNRS/UJF, B.P. 166, Grenoble, Cedex 09, 38042, France

    Carina Faber, Claudio Attaccalite, Valerio Olevano & Xavier Blase

  2. Laboratoire de Simulation Atomistique (L_Sim), SP2M, INAC, CEA-UJF, 17 Av. des Martyrs, Grenoble, 38054, France

    Ivan Duchemin & Thierry Deutsch

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  1. Carina Faber
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  2. Ivan Duchemin
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Correspondence to Xavier Blase.

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Faber, C., Duchemin, I., Deutsch, T. et al. Electron–phonon coupling and charge-transfer excitations in organic systems from many-body perturbation theory. J Mater Sci 47, 7472–7481 (2012). https://doi.org/10.1007/s10853-012-6401-7

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  • DOI: https://doi.org/10.1007/s10853-012-6401-7

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