Proceedings of nanoGe Fall Meeting19 (NFM19)
DOI: https://doi.org/10.29363/nanoge.nfm.2019.304
Publication date: 18th July 2019
Organic-inorganic metal-halide perovskites are emerging as one of the most important classes of optoelectronic materials. In addition to impressive photovoltaic performance (currently exceeding 24% power conversion efficiencies), three-dimensional (3D) and quasi-two dimensional (2D) layered halide perovskites are fast becoming highly attractive materials for application in lighting and lasing. In the context of these rapid developments, understanding the fundamental optoelectornic properties and photophysics of this complex class of materials is of key importance for future development of perovskite technologies. Furthermore, first principles computational methods provide an atomistic perspective into the optoelectronic properties of this novel class of materials and contribute to uncovering design rules and physical intuition that can guide future discoveries.
In this talk, we will present our recent work on understanding the electronic and optical properties of 3D inorganic lead-halide perovskites within many-body perturbation theory. In our calculations, we employ the GW approximation to calculate the quasiparticle band structure, and the Bethe-Salpeter equation to calculate excitonic spectra, while including the effect of spin-orbit coupling throughout. In this talk, we will briefly introduce the GW approximation and discuss in detail the quasiparticle band structure of CsPbX3, X=Cl, Br, I. Furthermore, we will discuss the Bethe-Salpeter formalism and present our calculations of the optical spectra and excitonic fine structure of 3D lead-halide perovskites. Finally, we will show how the excitonic structure of 3D lead-halide perovskites compares with the hydrogenic Wannier model and discuss more generally the role of lattice vibrations and dielectric screening for the excitonic properties of polar semiconductors.
This work is supported by the Department of Energy; computational resources provided by NERSC
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