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Collective chiroptical activity through the interplay of excitonic and charge-transfer effects in localized plasmonic fields

Author

Listed:
  • Huacheng Li

    (Donghua University
    Donghua University
    Donghua University)

  • Xin Xu

    (Donghua University
    Donghua University
    Donghua University)

  • Rongcheng Guan

    (Donghua University
    Donghua University
    Donghua University)

  • Artur Movsesyan

    (University of Electronic Science and Technology of China
    Ohio University)

  • Zhenni Lu

    (Donghua University
    Donghua University)

  • Qiliang Xu

    (Donghua University
    Donghua University)

  • Ziyun Jiang

    (Donghua University
    Donghua University
    Donghua University)

  • Yurong Yang

    (Donghua University
    Donghua University
    Donghua University)

  • Majid Khan

    (Donghua University
    Donghua University
    Donghua University)

  • Jin Wen

    (Donghua University
    Donghua University)

  • Hongwei Wu

    (Donghua University
    Donghua University)

  • Santiago Moya

    (Ciudad Universitaria s/n)

  • Gil Markovich

    (Tel Aviv University)

  • Huatian Hu

    (Istituto Italiano di Tecnologia)

  • Zhiming Wang

    (University of Electronic Science and Technology of China)

  • Qiang Guo

    (Peking University)

  • Tao Yi

    (Donghua University
    Donghua University)

  • Alexander O. Govorov

    (University of Electronic Science and Technology of China
    Ohio University)

  • Zhiyong Tang

    (National Center for Nanoscience and Technology
    University of Chinese Academy of Sciences)

  • Xiang Lan

    (Donghua University
    Donghua University
    Donghua University)

Abstract

The collective light-matter interaction of chiral supramolecular aggregates or molecular ensembles with confined light fields remains a mystery beyond the current theoretical description. Here, we programmably and accurately build models of chiral plasmonic complexes, aiming to uncover the entangled effects of excitonic correlations, intra- and intermolecular charge transfer, and localized surface plasmon resonances. The intricate interplay of multiple chirality origins has proven to be strongly dependent on the site-specificity of chiral molecules on plasmonic nanoparticle surfaces spanning the nanometer to sub-nanometer scale. This dependence is manifested as a distinct circular dichroism response that varies in spectral asymmetry/splitting, signal intensity, and internal ratio of intensity. The inhomogeneity of the surface-localized plasmonic field is revealed to affect excitonic and charge-transfer mixed intermolecular couplings, which are inherent to chirality generation and amplification. Our findings contribute to the development of hybrid classical-quantum theoretical frameworks and the harnessing of spin-charge transport for emergent applications.

Suggested Citation

  • Huacheng Li & Xin Xu & Rongcheng Guan & Artur Movsesyan & Zhenni Lu & Qiliang Xu & Ziyun Jiang & Yurong Yang & Majid Khan & Jin Wen & Hongwei Wu & Santiago Moya & Gil Markovich & Huatian Hu & Zhiming , 2024. "Collective chiroptical activity through the interplay of excitonic and charge-transfer effects in localized plasmonic fields," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-49086-3
    DOI: 10.1038/s41467-024-49086-3
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    References listed on IDEAS

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