Calculating the Circular Dichroism of Chiral Halide Perovskites: A Tight-Binding Approach

Sofia Apergi, Geert Brocks, Shuxia Tao (Corresponding author)

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Abstract

Chiral metal halide perovskites have emerged as promising optoelectronic materials for the emission and detection of circularly polarized visible light. Despite chirality being realized by adding chiral organic cations or ligands, the chiroptical activity originates from the metal halide framework. The mechanism is not well understood, as an overarching modeling framework is lacking. Capturing chirality requires going beyond electric dipole transitions, which is the common approximation in condensed matter calculations. We present a density functional theory (DFT) parametrized tight-binding (TB) model, which allows us to calculate optical properties including circular dichroism (CD) at low computational cost. Comparing Pb-based chiral perovskites with different organic cations and halide anions, we find that the structural helicity within the metal halide layers determines the size of the CD. Our results mark an important step in understanding the complex correlations of structural, electronic, and optical properties of chiral perovskites and provide a useful tool to predict new compounds with desired properties for novel optoelectronic applications.

Original languageEnglish
Pages (from-to)11565-11572
Number of pages8
JournalJournal of Physical Chemistry Letters
Volume14
Issue number51
DOIs
Publication statusPublished - 28 Dec 2023

Funding

The authors thank Mike Pols and Sander Driessen for their help in the analysis of the hydrogen bonding and optical properties associated with the chiral structures, respectively. S.A. acknowledges support from funding by NWO START-UP (Project No. 740.018.024) from The Netherlands. S.T. acknowledges funding by NWO START-UP (Project No. 740.018.024) and VIDI (Project No. VI.Vidi.213.091) from The Netherlands.

FundersFunder number
Nederlandse Organisatie voor Wetenschappelijk Onderzoek740.018.024

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