4.8 Article

High Throughput Mapping of Single Molecules' Redox Potentials on Electrode

Journal

ANALYTICAL CHEMISTRY
Volume 93, Issue 25, Pages 8864-8871

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.analchem.1c00984

Keywords

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Funding

  1. Office of Biological and Environmental Research, USA
  2. EMSL [50719]
  3. National Natural Science Foundation of China [32060521]
  4. Guilin University of Technology [RD18103020]
  5. Natural Science Foundation of Guangxi, China [2020GXNSFDA297023]

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By synchronizing electrochemical potential scanning with a single-molecule localization super-resolution fluorescence microscope, this study tracked kinetic fluorescence changes of hundreds of single molecular redox events simultaneously with high throughput. Through subsequent cross-correlation function analysis, the redox potentials of single molecules were mapped out in unprecedented detail from site to site in the imaging area. This work lays the foundation for mapping redox states at single-molecule levels in high throughput in chemical and biological systems.
By synchronizing electrochemical potential scanning with a single-molecule localization super-resolution fluorescence microscope, kinetic fluorescence changes of hundreds of single molecular redox events were tracked simultaneously with high throughput, and subsequent cross-correlation function analysis mapped single molecules' redox potentials (times) out on the imaging area from site to site in unprecedented detail by extracting electrochemically induced fluorescence change from apparently random fluorescence on/off blinking. This work paves the way toward mapping redox states at single-molecule levels in high throughput in chemical and biological systems.

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