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

Li, Shunran; Xu, Xian; Kocoj, Conrad A.; Zhou, Chenyu; Li, Yanyan; Chen, Du; Bennett, Joseph A.; Liu, Sunhao; Quan, Lina; Sarker, Suchismita; Liu, Mingzhao; Qiu, Diana Y.; Guo, Peijun

doi:10.1038/s41467-024-46851-2

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

Journal Article · Fri Mar 22 00:00:00 EDT 2024 · Nature Communications

DOI:https://doi.org/10.1038/s41467-024-46851-2· OSTI ID:2327035

;

; Li, Yanyan;

; Bennett, Joseph A.; Liu, Sunhao;

;

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.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0012704; AC02-05CH11231; AC05-00OR22725

OSTI ID:: 2327035

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 15 Journal Issue: 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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