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

Yongqing Yuan, Huacheng Li, Hao Yang, Cong Han, Huatian Hu, Alexander O. Govorov, Hao Yan, Xiang Lan

Research output: Contribution to journalArticlepeer-review

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.

Original languageEnglish (US)
Article numbere202210730
JournalAngewandte Chemie - International Edition
Volume61
Issue number44
DOIs
StatePublished - Nov 2 2022

Keywords

  • Chiral Plasmonic
  • DNA Self-Assembly
  • Multi-Scale
  • Nanoparticle Superstructure
  • Organic–Inorganic Hybrid

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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