Ag-DNA Emitter: Metal Nanorod or Supramolecular Complex?

作者:Ramazanov Ruslan R; Sych Tomash S; Reveguk Zakhar V; Maksimov Dmitriy A; Vdovichev Artem A; Kononov Alexei I*
来源:Journal of Physical Chemistry Letters, 2016, 7(18): 3560-3566.
DOI:10.1021/acs.jpclett.6b01672

摘要

Ligand-stabilized luminescent metal clusters, in particular, DNA-based Ag clusters, are now employed in a host of applications such as sensing and bioimaging. Despite their utility, the nature of their excited states as well as detailed structures of the luminescent metal-ligand complexes remain poorly understood. We apply a new joint experimental and theoretical approach based on QM/MM-MD simulations of the fluorescence excitation spectra for three Ag clusters synthesized on a 12-mer DNA. Contrary to a previously proposed "rod-like" model, our results. show that (1) three to four Ag atoms suffice to form a partially oxidized nanocluster emitting in visible range; (2) charge transfer from Ag cluster to DNA contributes to the excited states of the complexes; and (3) excitation spectra of the clusters are strongly affected by the bonding of Ag atoms to DNA bases. The presented approach can also provide a practical way to determine the structure and properties of other luminescent metal clusters.

  • 出版日期2016-9-15