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

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 Wang, Qiang Guo, Tao Yi, Alexander O. Govorov (), Zhiyong Tang and Xiang Lan ()
Additional contact information
Huacheng Li: Donghua University
Xin Xu: Donghua University
Rongcheng Guan: Donghua University
Artur Movsesyan: University of Electronic Science and Technology of China
Zhenni Lu: Donghua University
Qiliang Xu: Donghua University
Ziyun Jiang: Donghua University
Yurong Yang: Donghua University
Majid Khan: Donghua University
Jin Wen: Donghua University
Hongwei Wu: 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
Alexander O. Govorov: University of Electronic Science and Technology of China
Zhiyong Tang: National Center for Nanoscience and Technology
Xiang Lan: Donghua University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-49086-3

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