The predictive power of “one-shot” GW calculations for halide perovskites

ORAL

Abstract

Halide perovskites like the hybrid organic-inorganic APbX3 (A=CH3NH3+, CH(NH2)2+,... and X=I, Br, Cl) or the all-inorganic double perovskite Cs2BiAgBr6 are a class of compounds showing great promise as photovoltaic absorber materials. Accurately predicting their band gaps is challenging for first principles electronic structure methods because of the intricate coupling of structural and electronic degrees of freedom [1] as well as strong spin-orbit interactions. We use ab initio many-body perturbation theory, employing a “one-shot” G0W0 approach, to calculate the fundamental band gaps of experimentally characterized halide perovskites. We investigate the impact of the density functional theory starting point, pseudopotentials, and eigenvalue self-consistency on the calculated quasiparticle band gap. With our calculations, we assess whether there might be a “one size fits all” one-shot GW approach for this material class [2].

[1] L. Leppert, S. Reyes-Lillo, J. B. Neaton, J. Phys. Chem. Lett. 7, 3683 (2016). [2] L. Leppert, T. Rangel, J. Haber, J. B. Neaton, in preparation (2017).

*This work is supported by the Department of Energy, the Feodor-Lynen program of the Alexander von Humboldt foundation, and uses computational resources of NERSC.

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Presenters

  • Linn Leppert

    • Institute of Physics, University of Bayreuth
    • Physics, University of Bayreuth

Authors

  • Linn Leppert

    • Institute of Physics, University of Bayreuth
    • Physics, University of Bayreuth

  • Tonatiuh Rangel Gordillo

    • Lawrence Berkeley Natl Lab
    • Molecular Foundry, Lawrence Berkeley National Lab

  • Jonah Haber

    • Department of Physics, University of California Berkeley
    • Univ of California - Berkeley

  • Jeffrey Neaton

    • Molecular Foundry, Lawrence Berkeley National Laboratory; Department of Physics, University of California, Berkeley; Kavli Energy Nanosciences Institute at Berkeley
    • Physics, University of California, Berkeley; Lawrence Berkeley National Laboratory
    • Department of Physics, University of California
    • Univ of California - Berkeley
    • Lawrence Berkeley Natl Lab
    • Materials Science Division, Lawrence Berkeley National Laboratory
    • Molecular Foundry, Lawrence Berkeley National Lab
    • Physics, University of California, Berkeley
    • Department of Physics UCB; Molecular Foundry LBNL; Kavli ENSI
    • Lawrence Berkeley National Laboratory
    • Department of Physics, Univ of California - Berkeley
    • Lawrence Berkeley National Lab and University of California - Berkeley