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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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Circularly Polarized Light Emission From Single Chiral Hedgehog Particles Coated with Nanofilms of Achiral Perovskites
Abstract Metal‐halide perovskites are known for their strong and tunable luminescence. However, the synthesis of perovskite‐based particles with circularly polarized light emission (CPLE) remains challenging due to the complex interplay of metal‐ligand chemistries, crystallization patterns, and chirality transfer mechanisms. Achiral perovskites can be deposited on chiral “hedgehog” particles (CHIPs) with twisted spikes, producing chiroptically active materials with spectroscopic bands specific to the perovskite and chirality specific to the template CHIPs. Left‐ and right‐handed CPLE is engineered into complex particles comprised of a layer of perovskite deposited onto CHIPs coated with an intermediate silica layer. The spectral position of chiroptical bands, the optical asymmetryg‐factors, and single‐particle circularly polarized microscopy indicate that the observed CPLE is dominated by the post‐emission scattering from the twisted spikes of the parent particle. Templating luminescent nanofilms on CHIPs provides a simple pathway to a wide range of complex chiroptical materials; the dispersibility of the CHIPs in various solvents and the tunability of their chiral geometry enable their applications as single‐particle emitters with strong and controllable polarization rotation.
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- PAR ID:
- 10640188
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 37
- Issue:
- 45
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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