<p>Ultra-sensitive and specific biosensors capable of detecting low-concentration biomolecular interactions with the potential for simultaneous sensing of multiple analytes are still in demand and not achieved by conventional approaches. Traditional fluorescence-based biosensors have been plagued by low sensitivity, fouling by non-specific binding and an inability to multiplex with high precision in detection. This study approaches these challenges by developing a novel high-sensitivity plasmonic biosensor integrating plasmonic resonances with quantum dots (<i>QD</i>) photoluminescence. The five synergizing methods together propose biosensors that overcome the crucial limitations of the present technologies. First, the gap-tuned nanoplasmonic antenna arrays confine electromagnetic fields within sub-10&#xa0;mm gaps: amplifying quantum dots photoluminescence by ~ 15 × and detection limits as low as 1&#xa0;nM. Second, the gradient-alloyed core–shell quantum dot engineering enhances photoluminescence quantum yields up to ~ 85% and adjusts the energy transfer for Förster resonance energy transfer (FRET), showing a sensitivity of ~ 0.5&#xa0;nM. Third, angle-tuned plasmonic metasurfaces enable the multiplex detection of up to five analytes at a sensitivity of ~ 10&#xa0;nM by phase tuning the plasmonic resonances in concert with the quantum dots emissions. Fourth, zwitterionic functionalization proves to be very effective at reducing non-specific fouling (~ 95%), and thus detection specificity and reliability in complex biological samples are improved. Finally, second-harmonic generation (SHG)-enhanced plasmonic biosensing exhibits ultra-sensitive detection through non-linear optical effects, with detection limits ~ 0.01&#xa0;nM for DNA and pollutants. This proposed biosensor integrates the most advanced methods to provide unprecedented sensitivity and specificity levels of ~ 90–95% for multiplexing. This research opens up possibilities for next-generation biosensors with transformative applications in biomedical diagnostics and environmental monitoring processes.</p>

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Sensitivity Improved Plasmonic Biosensors with Coupling Quantum-Dots for Optimization of Biosensing Process: Application in Biomedical Diagnostics and Environmental Monitoring Processes

  • Ujwala S. Ghodeswar,
  • Kavita V. Joshi,
  • Manisha G. Waje,
  • Tejas R. Patil,
  • Sachin Upadhye,
  • Nilesh Shelke,
  • Haytham F. Isleem,
  • Pradeep Jangir,
  • Arpita,
  • Vikrant S. Vairagade

摘要

Ultra-sensitive and specific biosensors capable of detecting low-concentration biomolecular interactions with the potential for simultaneous sensing of multiple analytes are still in demand and not achieved by conventional approaches. Traditional fluorescence-based biosensors have been plagued by low sensitivity, fouling by non-specific binding and an inability to multiplex with high precision in detection. This study approaches these challenges by developing a novel high-sensitivity plasmonic biosensor integrating plasmonic resonances with quantum dots (QD) photoluminescence. The five synergizing methods together propose biosensors that overcome the crucial limitations of the present technologies. First, the gap-tuned nanoplasmonic antenna arrays confine electromagnetic fields within sub-10 mm gaps: amplifying quantum dots photoluminescence by ~ 15 × and detection limits as low as 1 nM. Second, the gradient-alloyed core–shell quantum dot engineering enhances photoluminescence quantum yields up to ~ 85% and adjusts the energy transfer for Förster resonance energy transfer (FRET), showing a sensitivity of ~ 0.5 nM. Third, angle-tuned plasmonic metasurfaces enable the multiplex detection of up to five analytes at a sensitivity of ~ 10 nM by phase tuning the plasmonic resonances in concert with the quantum dots emissions. Fourth, zwitterionic functionalization proves to be very effective at reducing non-specific fouling (~ 95%), and thus detection specificity and reliability in complex biological samples are improved. Finally, second-harmonic generation (SHG)-enhanced plasmonic biosensing exhibits ultra-sensitive detection through non-linear optical effects, with detection limits ~ 0.01 nM for DNA and pollutants. This proposed biosensor integrates the most advanced methods to provide unprecedented sensitivity and specificity levels of ~ 90–95% for multiplexing. This research opens up possibilities for next-generation biosensors with transformative applications in biomedical diagnostics and environmental monitoring processes.