The Institute of Chemistry, Center for Nanoscience and Nanotechnology, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.
Department of Applied Physics, Center for Nanoscience and Nanotechnology, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.
J Am Chem Soc. 2021 Oct 27;143(42):17622-17632. doi: 10.1021/jacs.1c07895. Epub 2021 Oct 13.
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/T, 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', the duplex L/T is separated, leading to the release of T and the formation of duplex L/L'. The released T leads to aggregation of the Au NPs or to the T-induced G-quadruplex bridged aggregated CdSe/ZnS QDs. Biocatalytic nicking of the L/L' duplex fragments L' and the released L displaces T 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.
介绍了导致金纳米粒子（NPs）或半导体量子点（QDs）的瞬态、耗散、聚集和去聚集以及对其瞬态光学性质进行控制的方法。该系统由核酸修饰的金 NPs 对或 CdSe/ZnS QDs 对、辅助双链 L/T 以及切口酶 Nt.BbvCI 作为功能模块组成，可产生 NPs 的瞬态聚集/去聚集并动态控制其光学性质。在燃料链 L'存在的情况下，双链 L/T 被分离，导致 T 的释放和双链 L/L'的形成。释放的 T 导致 Au NPs 的聚集或 T 诱导的 G-四链体桥接聚集 CdSe/ZnS QDs。L/L'双链片段 L'和释放的 L 的生物催化切口取代了桥接聚集的 NPs 或 QDs 的 T，导致原始 NPs 或 QDs 模块的动态恢复。Au NPs 的动态聚集/去聚集伴随着颗粒间等离子体耦合的瞬态光谱变化。CdSe/ZnS QDs 的动态聚集/去聚集通过以下方式探测：通过桥接 QDs 的血红素/G-四链体产生的瞬态化学发光以及在动态形成的 QDs 聚集体中进行的伴随的瞬态化学发光共振能量转移。还介绍了一个展示由核酸稳定的银纳米团簇（NCs）组成的反应模块的瞬态、耗散、发光性质的第三个系统。通过伴随切口过程的链置换，证明了超分子发光 Ag NCs 系统的瞬态动态形成和耗尽。
