In this work, Mn-doped AZIS/ZnS NCs were prepared using a nucleation doping approach with the tuning of Mn and Ag levels in their synthesis. The optical properties of Mn:AZIS/ZnS NCs are found to be significantly affected by Ag and Mn levels. Specifically, more Ag and Mn atoms in Mn:AZIS/ZnS NCs cause their fluorescence red-shift, and as the Ag or Mn level reaches a high threshold, the fluorescence lifetime of Mn:AZIS/ZnS NC has a significant drop. The reasons for the effects of Mn and Ag levels on NC optical properties were explored and discussed. Through this study, it is also found that with certain Ag and Mn levels in synthesis, some Mn:AZIS/ZnS NCs present optimal optical properties including high brightness (QY > 40%), long fluorescence lifetime (> 1.2 ms), low energy for excitation (excitable at 405 nm), and no reabsorption. The feasibility of the optimized NCs for time-gated fluorescence measurement using a portable/compact instrument was further demonstrated, which indicates the application potential of the NCs in time-gated biosensing including point-of-care testing. Notably, this study also discloses that Mn:AZIS/ZnS NCs with different lifetimes can be achieved by tuning Mn and Ag levels in synthesis, which may further broaden the applications of Mn:AZIS/ZnS NCs in multiplexing detection/measurement.
Recently, bright quantum dots (QDs) possessing low energy for excitation and long fluorescence lifetime in milliseconds have been reported. These QDs such as Mn doped I(II)-III-VI nanocrystals are promising for highly sensitive time-gated sensing applications with a portable or small benchtop “personal” instrument because their unique optical properties not only ensure a high signal-to-background ratio in time-gated fluorescence-intensity (TGFI) measurement but also significantly simplify the TGFI measurement instrument design criteria. In this work, following up the research progress on these QDs, we developed a compact TGFI measurement instrument with high sensitivity and cost-effectiveness for these QDs (more specifically Mn:AZIS/ZnS QDs) as signal reporters. We applied the instrument for sensitive detection of copper(ii) ions in highly autofluorescent rum (alcoholic beverage) in a fluorescence quenching assay utilizing these QDs for signal transduction. The results from this work suggest that this instrument together with bright QDs with low-energy for excitation and long fluorescence lifetimes should have potential to not only convert many regular (non-time-gated) QD-based fluorescence assays to time-gated assays for higher sensitivities or lower LODs, but also facilitate the development of highly sensitive assays for in-field or point-of-care testing.
In this work, a time-gated immunoassay platform using low-energy excitable and fluorescence long-lived Mn:AgZnInS/ZnS nanocrystals as signal transducers was developed and applied to the detection of the capsular polysaccharide (CPS) of Burkholderia pseudomallei, a Gram-negative bacterium that is the causative agent of melioidosis. CPS is a high molecular weight antigen displayed and is shed from the outer membrane of B. pseudomallei. The immunoassay using the time-gated platform presents a limit of detection at around 23 pg/ml when CPS is spiked in human serum.
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