Transient Dissipative Optical Properties of Aggregated Au Nanoparticles, CdSe/ZnS Quantum Dots, and Supramolecular Nucleic Acid-Stabilized Ag Nanoclusters

Transient, dissipative, aggregation and deaggregation of Au nanoparticles (NPs) or semiconductor quantum dots (QDs) leading to control over their transient optical properties are introduced. The systems consist of nucleic acid-modified pairs of Au NPs or pairs of CdSe/ZnS QDs, an auxiliary duplex L-1/T-1, and the nicking enzyme Nt.BbvCI as functional modules yielding transient aggregation/deaggregation of the NPs and dynamically controlling over their optical properties. In the presence of a fuel strand L-1', the duplex L-1/T-1 is separated, leading to the release of T-1 and the formation of duplex L-1/L-1'. The released T-1 leads to aggregation of the Au NPs or to the T-1-induced G-quadruplex bridged aggregated CdSe/ZnS QDs. Biocatalytic nicking of the L-1/L-1' duplex fragments L-1' and the released L-1 displaces T-1 bridging the aggregated NPs or QDs, resulting in the dynamic recovery of the original NPs or QDs modules. The dynamic aggregation/deaggregation of the Au NPs is followed by the transient interparticle plasmon coupling spectral changes. The dynamic aggregation/deaggregation of the CdSe/ZnS QDs is probed by following the transient chemiluminescence generated by the hemin/G-quadruplexes bridging the QDs and by the accompanying transient chemiluminescence resonance energy transfer proceeding in the dynamically formed QDs aggregates. A third system demonstrating transient, dissipative, luminescence properties of a reaction module consisting of nucleic acid-stabilized Ag nanoclusters (NCs) is introduced. Transient dynamic formation and depletion of the supramolecular luminescent Ag NCs system via strand displacement accompanied by a nicking process are demonstrated.

Automated summary

The study introduces a method to control the optical properties of Au NPs or CdSe/ZnS QDs through their dynamic aggregation/deaggregation, achieved by nucleic acid-modified pairs and biocatalytic reactions. It leads to the dynamic recovery of the original NP or QDs modules.