Large exchange-driven intrinsic circular dichroism of a chiral 2D hybrid perovskite

Shunran Li, Xian Xu, Conrad A. Kocoj, Chenyu Zhou, Yanyan Li, Du Chen, Joseph A. Bennett, Sunhao Liu, Lina Quan, Suchismita Sarker, Mingzhao Liu, Diana Y. Qiu () and Peijun Guo ()
Additional contact information
Shunran Li: Yale University
Xian Xu: Yale University
Conrad A. Kocoj: Yale University
Chenyu Zhou: Brookhaven National Laboratory
Yanyan Li: Yale University
Du Chen: Yale University
Joseph A. Bennett: Yale University
Sunhao Liu: Virginia Tech
Lina Quan: Virginia Tech
Suchismita Sarker: Cornell University
Mingzhao Liu: Brookhaven National Laboratory
Diana Y. Qiu: Yale University
Peijun Guo: Yale University

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract In two-dimensional chiral metal-halide perovskites, chiral organic spacers endow structural and optical chirality to the metal-halide sublattice, enabling exquisite control of light, charge, and electron spin. The chiroptical properties of metal-halide perovskites have been measured by transmissive circular dichroism spectroscopy, which necessitates thin-film samples. Here, by developing a reflection-based approach, we characterize the intrinsic, circular polarization-dependent complex refractive index for a prototypical two-dimensional chiral lead-bromide perovskite and report large circular dichroism for single crystals. Comparison with ab initio theory reveals the large circular dichroism arises from the inorganic sublattice rather than the chiral ligand and is an excitonic phenomenon driven by electron-hole exchange interactions, which breaks the degeneracy of transitions between Rashba-Dresselhaus-split bands, resulting in a Cotton effect. Our study suggests that previous data for spin-coated films largely underestimate the optical chirality and provides quantitative insights into the intrinsic optical properties of chiral perovskites for chiroptical and spintronic applications.

Date: 2024
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DOI: 10.1038/s41467-024-46851-2

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