Towards Bespoke Light-Matter Interactions in Heterogeneous Halide Perovskites from First Principles
Linn Leppert a
a University of Twente, MESA+ Institute for Nanotechnology, Netherlands
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting 2021 (NFM21)
#PerEmer21. Perovskites III: Emerging Materials and Phenomena
Online, Spain, 2021 October 18th - 22nd
Organizers: Moritz Futscher, Jovana Milic and Aditya Mohite
Invited Speaker, Linn Leppert, presentation 013
DOI: https://doi.org/10.29363/nanoge.nfm.2021.013
Publication date: 23rd September 2021

Organic-inorganic halide perovskites are record-breaking materials with a wide range of applications spanning photovoltaics, lighting, and detectors. These hybrid materials combine key properties of traditional inorganic semiconductors such as high carrier mobilities, with properties of organic semiconductors such as facile and low-cost synthesis. Single perovskites with stoichiometry ABX3 like the prototypical solar cell absorber CH3NH3PbI3 (MAPI) have excellent optoelectronic properties, but are hampered by instability, the toxicity of lead and scarcity of iodine. Furthermore, the ABX3 structural motif limits functionalization because only very few organic molecules fit into the A site cavity. New hybrid materials with alternative perovskite-like structural motifs vastly extend the chemical and structural diversity of this family of materials resulting in unusual and widely tuneable optoelectronic properties.

In this contribution I will demonstrate that it is the chemical and structural heterogeneity of such hybrid materials that determines their electronic and excited state properties. I will showcase first principles calculations - based on density functional theory and many-body perturbation theory - of several perovskite-type materials with optoelectronic properties significantly deviating from those of MAPI. Our calculations allow us to explore the atomistic origin of the unusual excited state properties of these materials and suggest routes for tuning them for tailored applications.

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