Orientation-Driven Chirality Funnels in Chiral Low-Dimensional Lead-Halide Perovskite Heterostructures [data]

DOI

Chiral hybrid metal-halide perovskites show low-symmetry crystal structures, large Rashba splitting, spin-filtering, and strong chiroptical activity. Circular dichroism and circularly polarized photoluminescence have been investigated in chiral perovskites with increasingly distorted chiral structures. Here, we report the fabrication of chiral (R/S)-EAPbI3 (EA = α-ethylbenzylamin) single crystals, which possess highly distorted octahedral structures with a high angle variance value of ~68 degree2. Using control in the fabrication conditions, we transfer chiral single crystals to thin films and achieve different crystal orientation preferences that induce tuneable chiroptical properties to their heterostructures with PbI2 nanodomains, which we characterize with in-situ X-ray diffraction and grazing-incidence wide-angle X-ray scattering measurements. Using transient chiroptical spectroscopies, we resolve photoexcited charge carrier dynamics and chirality transfer processes in such heterostructures down to cryogenic temperatures. We observe rapid carrier transfer along the in-plane (002) facets in chiral perovskite phases to PbI2 nanostructures within the initial few picoseconds, while carrier transfer along the out-of-plane (002) facets occurs at a slower rate. This fast transfer process leads to high photoluminescence intensities and large degrees of circular polarization in the emission from PbI2 nanodomains at cryogenic temperatures. Our findings report a multi-dimensional chiral-achiral heterostructure which takes advantage of controllable chirality transfer and offers new routes for future spintronic and chiroptical applications.

Identifier
DOI https://doi.org/10.11588/DATA/URBFPM
Related Identifier IsSupplementTo https://doi.org/10.1021/jacs.5c05172
Metadata Access https://heidata.uni-heidelberg.de/oai?verb=GetRecord&metadataPrefix=oai_datacite&identifier=doi:10.11588/DATA/URBFPM
Provenance
Creator Shangpu Liu ORCID logo; Jonathan Zerhoch ORCID logo; Markus W. Heindl (ORCID: 0000-0001-7968-617X); Chaoran Zhang; Tim Kodalle; Kun Sun; Andrii Shcherbakov ORCID logo; Stanislav Bodnar; Milon Miah; Mohammad Gholipoor; Christian Jandl; Alexander Pöthig; Joachim Ballmann; Ian D. Sharp; Peter Müller-Buschbaum; Carolin M. Sutter-Fella; Ulrich W. Paetzold; Felix Deschler
Publisher heiDATA
Contributor Felix Deschler
Publication Year 2025
Rights CC BY 4.0; info:eu-repo/semantics/openAccess; http://creativecommons.org/licenses/by/4.0
OpenAccess true
Contact Felix Deschler (Physikalisch-Chemisches Institut, Universität Heidelberg, Im Neuenheimer Feld 229, 69120 Heidelberg, Germany)
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Format application/pdf; application/octet-stream; text/plain
Size 1357137; 87508; 22322684; 81895; 62545; 103763; 4463293; 764645; 55675; 854636; 345981; 624299; 142455; 71322; 68485; 63832; 67267; 175979; 107610; 509425; 248764; 94596; 57548; 70663; 232884; 182638; 1681
Version 1.0
Discipline Chemistry; Engineering Sciences; Materials Science; Materials Science and Engineering; Natural Sciences; Physics