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PH-Driven Reversible Assembly and Disassembly of Colloidal Gold Nanoparticles.

ABSTRACT: Owing to the localized surface plasmon resonance (LSPR), dynamic manipulation of optical properties through the structure evolution of plasmonic nanoparticles has been intensively studied for practical applications. This paper describes a novel method for direct reversible self-assembly and dis-assembly of Au nanoparticles (AuNPs) in water driven by pH stimuli. Using 3-aminopropyltriethoxysilane (APTES) as the capping ligand and pH-responsive agent, the APTES hydrolyzes rapidly in response to acid and then condenses into silicon. On the contrary, the condensed silicon can be broken down into silicate by base, which subsequently deprotonates the APTES on AuNPs. By controlling condensation and decomposition of APTES, the plasmonic coupling among adjacent AuNPs could be reversible tuned to display the plasmonic color switching. This study provides a facile and distinctive strategy to regulate the reversible self-assembly of AuNPs, and it also offers a new avenue for other plasmonic nanoparticles to adjust plasmonic properties via reversible self-assembly.

SUBMITTER: Liu Y

PROVIDER: S-EPMC8116534 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Photon-to-matter chirality transfer offers both simplicity and universality to chiral synthesis, but its efficiency is typically low for organic compounds. Besides the fundamental importance of this process relevant for understanding the origin of homochirality on Earth, new pathways for imposing chiral bias during chemical process are essential for a variety of technologies from medicine to informatics. The strong optical activity of inorganic nanoparticles (NPs) affords photosynthetic routes to chiral superstructures using circularly polarized photons. Although plasmonic NPs are promising candidates for such synthetic routes due to the strong rotatory power of highly delocalized plasmonic states (Ma et al. Chem. Rev. 2017, 117 (12), 8041), realization of light-driven synthesis of chiral nanostructures has been more challenging for plasmonic NPs than for the semiconductor due to the short lifetime of the plasmonic states. Here we show that illumination of gold salt solutions with circularly polarized light induces the formation of NPs and their subsequent assembly into chiral nanostructures 10-15 nm in diameter. Despite their seemingly irregular shape, the resulting nanocolloids showed circular dichroism (CD) spectra with opposite polarity after exposure to photons with left and right circular polarization. The sign and spectral position of the CD peaks of illuminated dispersions matched those calculated for nanostructures with complex geometry identified from electron tomography images. Quantification of the complex shapes of NP assemblies using chirality measures revealed a direct correlation with the experimental spectra. The light-driven assembly of chiral nanostructures originates from the asymmetric displacement of NPs in dynamic assemblies by plasmonic fields followed by particle-to-particle attachment. The ability of gold NPs to "lock" the chirality of the incident photons in assembled nanostructures can be used to create a variety of chiral nanomaterials with plasmonic resonances.

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PH-Driven Reversible Assembly and Disassembly of Colloidal Gold Nanoparticles.

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