Enhanced Asymmetric\nCircularly Polarized Luminescence\nin Self-Organized Helical Superstructures Enabled by Macro-Chiral\nLiquid Crystal Quantum Dots

Circularly polarized luminescent (CPL) materials have\ngarnered\nconsiderable interest for a variety of advanced optical applications\nincluding 3D imaging, data encryption, and asymmetric catalysis. However,\nthe development of high-performance CPL has been hindered by the absence\nof simple synthetic methods for chiral luminescent emitters that exhibit\nboth high quantum yields and dissymmetry factors. In this study, we\npresent an innovative approach for the synthesis of macro-chiral liquid\ncrystal quantum dots (Ch-QDs/LC) and their CPL performance enhancement\nthrough doping with 4-cyano-4′-pentylbiphenyl (5CB), thus yielding\na CPL-emitting generator (CEG). The Ch-QDs/LCs were synthesized, and\ntheir surfaces functionalized with a chiral mesogenic ligand, specifically\ncholesteryl benzoate, anchored via a lipoic acid linker. Under the\nregulation of chiral 2S–Zn<sup>2+</sup> coordination complexes,\nthe chiral LC encapsulation process promotes coordinated ligand substitution,\nresulting in an exceptional quantum yield of 56.3%. This is accompanied\nby high absorption dissymmetry factor (<i>g</i><sub>abs</sub>) and luminescence dissymmetry factor (<i>g</i><sub>lum</sub>) values ranging from 10<sup>–3</sup> to 10<sup>–2</sup>, surpassing most reported dissymmetry factors by at least an order\nof magnitude. The modular Ch-QDs/LCs demonstrate the ability to transfer\nchirality to the surrounding medium efficiently and manifest macro-chiral\ncharacteristics within a nematic LC matrix. Utilizing Ch-QDs/LC as\nan effective CPL emitter within achiral 5CB matrices enabled the system\nto achieve a maximum <i>g</i><sub>lum</sub> value of 0.35.\nThe resultant CEG device acted as a direct CPL source, initiating\nenantioselective photopolymerization.

Publication Details

Journal
Figshare
Published
2024-11-04
DOI
https://doi.org/10.1021/acsnano.4c10423.s001
Primary Topic
Synthesis and Properties of Aromatic Compounds
Type
article
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article

Enhanced Asymmetric\nCircularly Polarized Luminescence\nin Self-Organized Helical Superstructures Enabled by Macro-Chiral\nLiquid Crystal Quantum Dots

Figshare
Synthesis and Properties of Aromatic Compounds
article

Enhanced Asymmetric\nCircularly Polarized Luminescence\nin Self-Organized Helical Superstructures Enabled by Macro-Chiral\nLiquid Crystal Quantum Dots

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Abstract

Circularly polarized luminescent (CPL) materials have\ngarnered\nconsiderable interest for a variety of advanced optical applications\nincluding 3D imaging, data encryption, and asymmetric catalysis. However,\nthe development of high-performance CPL has been hindered by the absence\nof simple synthetic methods for chiral luminescent emitters that exhibit\nboth high quantum yields and dissymmetry factors. In this study, we\npresent an innovative approach for the synthesis of macro-chiral liquid\ncrystal quantum dots (Ch-QDs/LC) and their CPL performance enhancement\nthrough doping with 4-cyano-4′-pentylbiphenyl (5CB), thus yielding\na CPL-emitting generator (CEG). The Ch-QDs/LCs were synthesized, and\ntheir surfaces functionalized with a chiral mesogenic ligand, specifically\ncholesteryl benzoate, anchored via a lipoic acid linker. Under the\nregulation of chiral 2S–Zn<sup>2+</sup> coordination complexes,\nthe chiral LC encapsulation process promotes coordinated ligand substitution,\nresulting in an exceptional quantum yield of 56.3%. This is accompanied\nby high absorption dissymmetry factor (<i>g</i><sub>abs</sub>) and luminescence dissymmetry factor (<i>g</i><sub>lum</sub>) values ranging from 10<sup>–3</sup> to 10<sup>–2</sup>, surpassing most reported dissymmetry factors by at least an order\nof magnitude. The modular Ch-QDs/LCs demonstrate the ability to transfer\nchirality to the surrounding medium efficiently and manifest macro-chiral\ncharacteristics within a nematic LC matrix. Utilizing Ch-QDs/LC as\nan effective CPL emitter within achiral 5CB matrices enabled the system\nto achieve a maximum <i>g</i><sub>lum</sub> value of 0.35.\nThe resultant CEG device acted as a direct CPL source, initiating\nenantioselective photopolymerization.

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Synthesis and Properties of Aromatic Compounds
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