Early‐stage detection of diseases caused by pathogens is a prerequisite for expedient patient care. Due to the limited signal‐to‐noise ratio, molecular diagnostics needs molecular signal amplification after recognition of the target molecule. In this present study, we demonstrate the design of plasmonically coupled bimetallic Ag coated Au nanostar dimers with controlled nanogap using rectangular DNA origami. We further report the utility of the designed nanostar dimer structures as efficient SERS substrate for the ultrasensitive and label‐free detection of the pyocyanin molecule, which is a biomarker of the opportunistic pathogenic bacteria, Pseudomonas aeruginosa. The experimental results showed that the detection limit of pyocyanin with such nanoantenna based biosensor was 335 pM, which is much lower than the clinical range of detection. Thus, fast, sensitive and label‐free detection of pyocyanin at ultralow concentration in an infected human body can pave a facile route for early stage warning for severe bacterial infections.
Engineering hotspots in surface-enhanced
Raman spectroscopy (SERS)
through precisely controlled assembly of plasmonic nanostructures
capable of expanding intense field enhancement are highly desirable
to enhance the potentiality of SERS as a label-free optical tool for
single molecule detection. Inspired by DNA origami technique, we constructed
plasmonic dimer nanoantennas with a tunable gap decorated with Ag-coated
Au nanostars on origami. Herein, we demonstrate the single-molecule
SERS enhancements of three dyes with emission in different spectral
regions after incorporation of single dye molecules in between two
nanostars. The enhancement factors (EFs) achieved in the range of
109–1010 for all the single dye molecules,
under both resonant and nonresonant excitation conditions, would enable
enhanced photostability during time-series measurement. We further
successfully explored the potential of our designed nanoantennas to
accommodate and detect a single thrombin protein molecule after selective
placement in the wide nanogap of 10 nm. Our results suggest that such
nanoantennas can serve as a broadband SERS enhancer and enable specific
detection of target biological molecules with single-molecule sensitivity.
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