Department of Materials Science and Engineering, University of California, Irvine, California 92697, United States.
Nanoscience Center and Department of Chemistry, University of Copenhagen, Universitetsparken 5, 2100 Copenhagen, Denmark.
J Phys Chem Lett. 2022 Sep 8;13(35):8305-8311. doi: 10.1021/acs.jpclett.2c02207. Epub 2022 Aug 29.
DNA oligomers are known to serve as stabilizing ligands for silver nanoclusters (Ag-DNAs) with rod-like nanocluster geometries and nanosecond-lived fluorescence. Here, we report two Ag-DNAs that possess distinctly different structural properties and are the first to exhibit only microsecond-lived luminescence. These emitters are characterized by significant broadband downconversion from the ultraviolet/visible to the near-infrared region. Circular dichroism spectroscopy shows that the structures of these two Ag-DNAs differ significantly from previously reported Ag-DNAs. We find that these nanoclusters contain eight valence electrons, making them the first reported DNA-stabilized luminescent quasi-spherical superatoms. This work demonstrates the important role that nanocluster composition and geometry play in dictating luminescence properties of Ag-DNAs and significantly expands the space of structure-property relations that can be achieved for Ag-DNAs.
DNA 寡聚物已知可作为棒状纳米团簇几何形状和纳秒寿命荧光的银纳米团簇 (Ag-DNAs) 的稳定配体。在这里,我们报告了两种具有明显不同结构特性的 Ag-DNAs,它们是第一个表现出仅微秒寿命发光的 Ag-DNAs。这些发射器的特点是从紫外/可见到近红外区域的显著宽带下转换。圆二色性光谱表明,这两种 Ag-DNAs 的结构与以前报道的 Ag-DNAs 有很大的不同。我们发现这些纳米团簇含有 8 个价电子,这使它们成为第一个报道的 DNA 稳定发光准球形超原子。这项工作表明了纳米团簇组成和几何形状在决定 Ag-DNAs 发光性质中的重要作用,并显著扩展了可以实现的 Ag-DNAs 的结构-性质关系的空间。