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    Reactive-Oxygen-Species-Mediated Surface Oxidation of Single-Molecule DNA Origami by an Atomic Force Microscope Tip-Mounted C-60 Photocatalyst

    Year: 2021

    Journal: ACS Nano, Volume 15, DEC 28, page 19256–19265

    Authors: Ray, Ankita; Passiu, Cristiana; Nasuda, Masayuki; Ramakrishna, Shivaprakash N.; Rossi, Antonella; Kuzuya, Akinori; Spencer, Nicholas D.; Yamakoshi, Yoko

    Organizations: SNF [200021_156097]; ETH [ETH-45 19-1]

    Keywords: atomic force microscope; reactive oxygen species; singlet oxygen; DNA origami; C-60 photocatalyst; single molecule

    A tripod molecule incorporating a C-60 photocatalyst into a rigid scaffold with disulfide legs was designed and synthesized for the stable and robust attachment of C-60 onto an Au-coated atomic force microscope (AFM) tip. The tripod-C-60 was immobilized onto the tip by forming S-Au bonds in the desired orientation and a dispersed manner, rendering it suitable for the oxidation and scission of single molecules on a countersurface, thereby functioning as molecular shears. A DNA origami with a well-defined structure was chosen as the substrate for the tip-induced oxidation. The gold-coated, C-60-functionalized AFM tip was used for both AFM imaging and oxidation of DNA origami upon visible-light irradiation. The localized and temporally controlled oxidative damage of DNA origami was successfully performed at the single-molecule level via singlet-oxygen (O-1(2)) generation from the immobilized C-60 on the AFM tip. This oxidative damage to DNA origami can be carried out under ambient conditions in a fluid cell at room temperature, rendering it well-suited for the manipulation of a variety of species on surfaces via a spatially and temporally controlled oxidation reaction triggered by O-1(2) locally generated from the immobilized C-60 on the AFM tip.
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