Volume 61, Issue 44 e202210730
Research Article

Unraveling the Complex Chirality Evolution in DNA-Assembled High-Order, Hybrid Chiroplasmonic Superstructures from Multi-Scale Chirality Mechanisms

Yongqing Yuan

Yongqing Yuan

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Center for Advanced Low-dimension Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620 China

These authors contributed equally to this work.

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Huacheng Li

Huacheng Li

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Center for Advanced Low-dimension Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620 China

These authors contributed equally to this work.

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Hao Yang

Hao Yang

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Center for Advanced Low-dimension Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620 China

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Cong Han

Cong Han

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Center for Advanced Low-dimension Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620 China

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Prof. Huatian Hu

Prof. Huatian Hu

Hubei Key Laboratory of Optical Information and Pattern Recognition, Wuhan Institute of Technology, Wuhan, Hubei 430205 China

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Prof. Dr. Alexander O. Govorov

Prof. Dr. Alexander O. Govorov

Department of Physics and Astronomy and the Nanoscale & Quantum Phenomena Institute, Ohio University, Athens, OH 45701 USA

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Prof. Hao Yan

Prof. Hao Yan

Center for Molecular Design and Biomimetics, The Biodesign Institute, School of Molecular Sciences, Arizona State University, Tempe, AZ 85287 USA

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Prof. Xiang Lan

Corresponding Author

Prof. Xiang Lan

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Center for Advanced Low-dimension Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620 China

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First published: 09 September 2022
Citations: 15

Graphical Abstract

Multi-scale chirality evolution was observed from DNA-assembled hybrid chiroplasmonic superstructures comprised of metal nanoparticles and organic chromophores, as a result of distinct fundamental chiral interactions at different hierarchical levels. The findings present new challenges to current theoretical frameworks to describe chiral hybrid systems, and will motivate computational and theoretical advances.

Abstract

Hierarchical, chiral hybrid superstructures of chromophores and nanoparticles are expected to give rise to intriguing unveiled chiroptical responses originating from the complex chiral interactions among the components. Herein, DNA origami cavity that could self-assemble into one-dimensional (1D) DNA tubes was employed as a scaffold to accurately organize metal nanoparticles and chromophores. The chiral interactions were studied at the level of individual hybrid particles and their 1D hybrid superstructures. Complex chirality mechanisms involving global structural chirality, plasmon-induced circular dichroism (PICD) and exciton-coupled circular dichroism (ECCD) were disentangled. The multiplexed CD spectrum superposition revealed the chirality evolution at different length scales. These results can offer a model for boosting the theoretical understanding of classical-quantum hybrid systems, and would inspire the future design of optically-active substances across length scales.

Conflict of interest

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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