Autonomous DNA Nanoswitch Encodes Quantum-Yield Oscillations for Time-Resolved Single-Molecule Readout
Precise control of fluorescence quantum yield at the single-emitter level is pivotal for molecular imaging and ultrasensitive detection, yet most plasmon-fluorophore studies rely on fixed gaps or ensemble averages, leaving autonomous, real-time tuning of an individual emitter via nanometal surface energy transfer largely unexplored. Here, we introduce an autonomous DNA-metallic nanoswitch that continuously modulates a single emitter's quantum yield by dynamically varying its separation from a gold nanoparticle. Programmable DNA hybridization acts as a molecular lever that shuttles the dye between a subnanometer "off" state (<i>r</i> < 1 nm), where nonradiative energy transfer quenches emission, and a multinanometer "on" state (<i>r</i> > 4 nm), where emission recovers; the resulting reversible oscillations follow the characteristic ∼1/d<sup>4</sup> distance dependence. This distance-encoded operation yields robust self-blinking trajectories and time-domain metrics (on/off contrast and dwell times) even under high-background conditions. With built-in blinking, nanometer-scale positioning, and straightforward DNA addressability, the nanoswitch deepens understanding of metal-fluorophore coupling and provides a versatile platform for time-resolved single-molecule readout in imaging and diagnostics.
Authors
- N. Zhang
- Peng Zheng (ORCID: https://orcid.org/0000-0001-5907-8505)
- Tao Ding (ORCID: https://orcid.org/0000-0001-8903-612X)
- Haodong Li (ORCID: https://orcid.org/0009-0000-5822-7353)
- Min Ke
- Le Liang
- Hongyue Hu
Institutions
- Johns Hopkins University (US)
- Wuhan University (CN)
- Zhongnan Hospital of Wuhan University (CN)
Publication Details
- Journal
- Analytical Chemistry
- Published
- 2026-02-03
- DOI
- https://doi.org/10.1021/acs.analchem.5c06635
- Primary Topic
- Advanced biosensing and bioanalysis techniques
- Type
- article
- Field-Weighted Citation Impact
- 0.00