4.8 Article

Plasmon Coupling in DNA-Assembled Silver Nanoclusters

Journal

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 36, Pages 14573-14580

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c04949

Keywords

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Funding

  1. National Institutes of Health [GM079359, CA133086]
  2. NSFC [21505032, 21325520, 1327009]

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The research indicates that the absorption peaks of DNA-templated Ag nanoclusters are sensitive to the assembled distances and exhibit characteristics of plasmon coupling; TDDFT simulations suggest that the absorption originates from plasmons, and the consistent trend between experimental and simulation results implies the possibility of plasmon coupling. DNA-AgNCs have the potential to be promising materials for constructing plasmon-coupling devices with ultra-small size, site-specific and stoichiometric binding abilities, and biocompatibility.
Quantum-size metal clusters with multiple delocalized electrons could support collective plasmon excitation, and thus, theoretically, coupling of plasmons in the few-atom limit might exist between assembled metal clusters, while currently few experimental observations about this phenomenon have been reported. Here we examined the optical absorption of DNA-templated Ag nanoclusters (DNA-AgNCs) assembled through DNA hybridization and found their absorption peaks were sensitive to the assembled distances, which share common characteristics with classical plasmon coupling. Dipolar charge distribution, multiple transition contributed optical absorption, and strongly enhanced electric field simulated by time-dependent density functional theory (TDDFT) indicated the origin of the absorption of individual DNA-AgNCs is a plasmon. The consistency of the peak-shifting trend between experimental and simulation results for assembled DNA-AgNCs suggested the possible presence of plasmon coupling. Our data imply the possibility for quantum-size structures to support plasmon coupling and also show that DNA-AgNCs possess the potential to be promising materials for construction of plasmon-coupling devices with ultrasmall size, sitespecific and stoichiometric binding abilities, and biocompatibility.

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