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

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dc.contributor.authorLi, Shunranen
dc.contributor.authorXu, Xianen
dc.contributor.authorKocoj, Conrad A.en
dc.contributor.authorZhou, Chenyuen
dc.contributor.authorLi, Yanyanen
dc.contributor.authorChen, Duen
dc.contributor.authorBennett, Joseph A.en
dc.contributor.authorLiu, Sunhaoen
dc.contributor.authorQuan, Linaen
dc.contributor.authorSarker, Suchismitaen
dc.contributor.authorLiu, Mingzhaoen
dc.contributor.authorQiu, Diana Y.en
dc.contributor.authorGuo, Peijunen
dc.date.accessioned2025-02-17T17:39:10Zen
dc.date.available2025-02-17T17:39:10Zen
dc.date.issued2024-03-22en
dc.description.abstractIn 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.en
dc.description.versionPublished versionen
dc.format.extent9 page(s)en
dc.format.mimetypeapplication/pdfen
dc.identifierARTN 2573 (Article number)en
dc.identifier.doihttps://doi.org/10.1038/s41467-024-46851-2en
dc.identifier.eissn2041-1723en
dc.identifier.issn2041-1723en
dc.identifier.issue1en
dc.identifier.orcidQuan, Lina [0000-0001-9301-3764]en
dc.identifier.other10.1038/s41467-024-46851-2 (PII)en
dc.identifier.pmid38519487en
dc.identifier.urihttps://hdl.handle.net/10919/124602en
dc.identifier.volume15en
dc.language.isoenen
dc.publisherNature Portfolioen
dc.relation.urihttps://www.ncbi.nlm.nih.gov/pubmed/38519487en
dc.rightsCreative Commons Attribution 4.0 Internationalen
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/en
dc.titleLarge exchange-driven intrinsic circular dichroism of a chiral 2D hybrid perovskiteen
dc.title.serialNature Communicationsen
dc.typeArticle - Refereeden
dc.type.dcmitypeTexten
dc.type.otherArticleen
dc.type.otherJournalen
dcterms.dateAccepted2024-03-12en
pubs.organisational-groupVirginia Techen
pubs.organisational-groupVirginia Tech/Scienceen
pubs.organisational-groupVirginia Tech/Science/Chemistryen
pubs.organisational-groupVirginia Tech/All T&R Facultyen
pubs.organisational-groupVirginia Tech/Science/COS T&R Facultyen

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