Collective chiroptical activity through the interplay of excitonic and charge-transfer effects in localized plasmonic fields.
Autor: | Li H; State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, 201620, Shanghai, China.; Center for Advanced Low-dimension Materials, Donghua University, 201620, Shanghai, China.; College of Materials Science and Engineering, Donghua University, 201620, Shanghai, China., Xu X; State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, 201620, Shanghai, China.; Center for Advanced Low-dimension Materials, Donghua University, 201620, Shanghai, China.; College of Materials Science and Engineering, Donghua University, 201620, Shanghai, China., Guan R; State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, 201620, Shanghai, China.; Center for Advanced Low-dimension Materials, Donghua University, 201620, Shanghai, China.; College of Materials Science and Engineering, Donghua University, 201620, Shanghai, China., Movsesyan A; Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, 610054, Chengdu, China.; Department of Physics and Astronomy and Nanoscale and Quantum Phenomena Institute, Ohio University, Athens, OH, 45701, USA., Lu Z; State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, 201620, Shanghai, China.; College of Chemistry and Chemical Engineering, Donghua University, 201620, Shanghai, China., Xu Q; State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, 201620, Shanghai, China.; College of Chemistry and Chemical Engineering, Donghua University, 201620, Shanghai, China., Jiang Z; State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, 201620, Shanghai, China.; Center for Advanced Low-dimension Materials, Donghua University, 201620, Shanghai, China.; College of Materials Science and Engineering, Donghua University, 201620, Shanghai, China., Yang Y; State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, 201620, Shanghai, China.; Center for Advanced Low-dimension Materials, Donghua University, 201620, Shanghai, China.; College of Materials Science and Engineering, Donghua University, 201620, Shanghai, China., Khan M; State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, 201620, Shanghai, China.; Center for Advanced Low-dimension Materials, Donghua University, 201620, Shanghai, China.; College of Materials Science and Engineering, Donghua University, 201620, Shanghai, China., Wen J; State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, 201620, Shanghai, China.; College of Materials Science and Engineering, Donghua University, 201620, Shanghai, China., Wu H; State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, 201620, Shanghai, China.; College of Chemistry and Chemical Engineering, Donghua University, 201620, Shanghai, China., de la Moya S; Departamento de Química Orgánica, Facultad de Ciencias Químicas, Universidad Complutense de Madrid, Ciudad Universitaria s/n, 28040, Madrid, Spain., Markovich G; School of Chemistry, Raymond and Beverly Sackler Faculty of Exact Sciences, Tel Aviv University, Tel Aviv, 69978, Israel., Hu H; Center for Biomolecular Nanotechnologies, Istituto Italiano di Tecnologia, Via Barsanti 14, Arnesano, 73010, LE, Italy., Wang Z; Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, 610054, Chengdu, China., Guo Q; State Key Laboratory of Protein and Plant Gene Research, Center for Life Sciences, Academy for Advanced Interdisciplinary Studies, School of Life Sciences, Peking University, 100871, Beijing, China., Yi T; State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, 201620, Shanghai, China.; College of Chemistry and Chemical Engineering, Donghua University, 201620, Shanghai, China., Govorov AO; Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, 610054, Chengdu, China. govorov@ohio.edu.; Department of Physics and Astronomy and Nanoscale and Quantum Phenomena Institute, Ohio University, Athens, OH, 45701, USA. govorov@ohio.edu., Tang Z; CAS Key Laboratory of Nanosystem and Hierarchical Fabrication & CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, 100190, Beijing, China.; University of Chinese Academy of Sciences, 100049, Beijing, China., Lan X; State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, Donghua University, 201620, Shanghai, China. xlan@dhu.edu.cn.; Center for Advanced Low-dimension Materials, Donghua University, 201620, Shanghai, China. xlan@dhu.edu.cn.; College of Materials Science and Engineering, Donghua University, 201620, Shanghai, China. xlan@dhu.edu.cn. |
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Jazyk: | angličtina |
Zdroj: | Nature communications [Nat Commun] 2024 Jun 06; Vol. 15 (1), pp. 4846. Date of Electronic Publication: 2024 Jun 06. |
DOI: | 10.1038/s41467-024-49086-3 |
Abstrakt: | 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. (© 2024. The Author(s).) |
Databáze: | MEDLINE |
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