Optoelectronic Properties of Halide Perovskites with ab Initio Many-body Perturbation Theory

Linn Leppert^a

^aInstitute of Physics, University of Bayreuth, Germany, Bayreuth, Germany

Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting19 (NFM19)

#PERFuDe19. Halide perovskites: when theory meets experiment from fundamentals to devices

Berlin, Germany, 2019 November 3rd - 8th

Organizers: Claudine Katan, Wolfgang Tress and Simone Meloni

Oral, Linn Leppert, presentation 074
DOI: https://doi.org/10.29363/nanoge.nfm.2019.074
Publication date: 18th July 2019

Halide perovskites are a broad class of compounds featuring 3D materials like the hybrid organic-inorganic CH₃NH₃PbI₃ and the all-inorganic double perovskite Cs₂BiAgBr₆, 2D layered Ruddlesden-Popper perovskites [1], quasi-0D materials like Cs₃Bi₂I₉, and many more. They have shown great promise for photovoltaic applications with power conversion efficiencies of perovskite-based solar cells exceeding 23%. Accurately predicting their fundamental band gaps and excited state properties is challenging for first principles electronic structure methods because of the intricate coupling of structural and electronic degrees of freedom [2, 3], strong spin-orbit interactions, and the existence of strongly bound excitons in low-dimensional systems. In this contribution, I will discuss our recent progress in describing the optoelectronic properties of halide perovskites using Green’s function-based many-body perturbation theory. We investigate the predictive power of “one-shot” G₀W₀ calculations, with a focus on the impact of the density functional theory starting point, pseudopotentials, eigenvalue self-consistency, and the perovskite structure [4]. With our calculations, we assess whether there might be a “one size fits all” one-shot GW approach for this material class. Our findings have severe repercussions for the calculation of complex doped and defected systems [5], as well as for the calculation of excited states and exciton binding energies.

References:

[1] Connor, B. A.; Leppert, L.; Smith, M.; Neaton, J. B.; Karunadasa, H. I. Layered Halide Double Perovskites: Dimensional Reduction of Cs2AgBiBr6. J. Am. Chem. Soc. 2018, 140, 5235.

[2] Leppert, L.; Reyes-Lillo, S. E.; Neaton; J. B. Electric Field- and Strain-Induced Rashba Effect in Hybrid Halide Perovskites. J. Phys. Chem. Lett. 2016, 7, 3683.

[3] Leblebici, S. Y.; Leppert, L.; Li, Y.; Reyes-Lillo, S. E.; Wickenburg, S.; Wong, E.; Lee, J.; Melli, M.; Ziegler, D.; Angell, D. K.; Ogletree, D. F.; Ashby, P. D.; Toma, F. M.; Neaton, J. B.; Sharp, I. D.; Weber-Bargioni, A. Facet-dependent photovoltaic efficiency variations in single grains of hybrid halide perovskite. Nature Energy 2016, 1, 16093.

[4] Slavney, A. H.; Leppert, L.; Saldivar Valdes, A.; Bartesaghi; D.; Savenije, T. J.; Neaton, J. B.; Karunadasa, H. I. Small-Bandgap Halide Double Perovskites. Angew. Chem. Int. Ed. 2018, 57, 12765.

[5] Slavney, A. H.; Leppert, L.; Bartesaghi, D.; Gold-Parker, A.; Toney, M. F.; Savenije, T. J.; Neaton, J. B.; Karunadasa, H. I. Defect-Induced Band-Edge Reconstruction of a Bismuth-Halide Double Perovskite for Visible-Light Absorption. 2017, 139, 5015.

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