Optical Properties of Organometallic Perovskite: An ab initio Study using Relativistic GW Correction and Bethe-Salpeter Equation

Abstract

In the development of highly efficient photovoltaic cells, solid perovskite systems have demonstrated unprecedented promise, with the figure of merit exceeding nineteen percent of efficiency. In this paper, we investigate the optical and vibrational properties of organometallic cubic perovskite CH3NH3PbI3 using first-principles calculations. For accurate theoretical description, we go beyond conventional density functional theory (DFT), and calculated optical conductivity using relativist quasi-particle (GW) correction. Incorporating these many-body effects, we further solve Bethe-Salpeter equations (BSE) for excitons, and found enhanced optical conductivity near the gap edge. Due to the presence of organic methylammonium cations near the center of the perovskite cell, the system is sensitive to low energy vibrational modes. We estimate the phonon modes of CH3NH3PbI3 using small displacement approach, and further calculate the infrared absorption (IR) spectra. Qualitatively, our calculations of low-energy phonon frequencies are in good agreement with our terahertz measurements. Therefore, for both energy scales (around 2 eV and 0-20 meV), our calculations reveal the importance of many-body effects and their contributions to the desirable optical properties in the cubic organometallic perovskites system.

arXiv comment5 pages, 4 figures

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Cited by in corpus (10)

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• Role of Polar Phonons in the Photo Excited State of Metal Halide Perovskites
• Atomic structure of metal-halide perovskites from first principles: The chicken-and-egg paradox of the organic-inorganic interaction
• Modelization of charge carriers mobilities in halide perovskites: Fröhlich scattering and quantum localization effects in a dynamic disorder regime
• Elucidating the role of Sn-substitution and Pb-$\square$ in regulating stability and carrier concentration in CH${}_3$NH${}_3$Pb${}_{1-X-Y}$Sn${}_X$${\square }_Y$I${}_3$
• Aziridinium lead iodide: a stable, low bandgap hybrid halide perovskite for photovoltaics
• Exciton-Dominated Core-Level Absorption Spectra of Hybrid Organic-Inorganic Lead Halide Perovskites
• Breathing bands due to molecular order in CH3NH3PbI3
• On the Adsorption Mechanism of Caffeine on MAPbI3 Perovskite Surfaces: A Combined UMC--DFT Study
• Free-electron effects on optical absorption of hybrid perovskite CH${}_3$NH${}_3$PbI${}_3$ from first principles