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Abstract Translation of chirality and asymmetry across structural motifs and length scales plays a fundamental role in nature, enabling unique functionalities in contexts ranging from biological systems to synthetic materials. Here, we introduce a structural chirality transfer across the organic–inorganic interface in two-dimensional hybrid perovskites using appropriate chiral organic cations. The preferred molecular configuration of the chiral spacer cations, R -(+)- or S -(−)-1-(1-naphthyl)ethylammonium and their asymmetric hydrogen-bonding interactions with lead bromide-based layers cause symmetry-breaking helical distortions in the inorganic layers, otherwise absent when employing a racemic mixture of organic spacers. First-principles modeling predicts a substantial bulk Rashba-Dresselhaus spin-splitting in the inorganic-derived conduction band with opposite spin textures between R - and S -hybrids due to the broken inversion symmetry and strong spin-orbit coupling. The ability to break symmetry using chirality transfer from one structural unit to another provides a synthetic design paradigm for emergent properties, including Rashba-Dresselhaus spin-polarization for hybrid perovskite spintronics and related applications.
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Chiral photon emission from a chiral–achiral perovskite heterostructure
Chiral semiconductors have been recently suggested as the basic building blocks for the design of chiral optoelectronic and electronic devices for chiral emission and spintronics. Herein, we report that through the formation of a chiral/achiral heterostructure, one can develop a chiral system that integrates the merits of both chiral and achiral components for developing a demanded chiral emitter. In the R-(+)-(or S-(−)-)1-(1-naphthyl)-ethylammonium lead bromide/CsPbBr3 heterostructure, we show that the photoluminescence of CsPbBr3 carries a degree of circular polarization of around 1% at room temperature. It is explained that such chiral emission is enabled through the chiral self-trapped exitonic absorption of R-(+)- (or S-(−)-)1-(1-naphthyl)-ethylammonium lead bromide. This work may provide an alternative way to generate bright circularly polarized light from achiral materials, which has potential applications in spintronics, biosensing, and signal encryption.
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- Award ID(s):
- 2024972
- PAR ID:
- 10562941
- Publisher / Repository:
- AIP
- Date Published:
- Journal Name:
- Applied Physics Letters
- Volume:
- 124
- Issue:
- 11
- ISSN:
- 0003-6951
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript
- Journal Article:
- https://doi.org/10.1063/5.0180188
