In this work, an ultrasensitive fluorescence strategy on counting the degree of aggregation (DOA) of QDs aggregates was developed for Hg2+ detection, which is based on thymine-Hg2+-thymine (T-Hg2+-T) coordination chemistry. Oligonucleotides containing 12 thymines are modified on the surface of QDs which could protect QDs effectively from aggregation in the absence of Hg2+. While in the presence of Hg2+, QDs will be made to attach with each other by the structure of “T-Hg2+-T” formed, and then aggregated in the sensing system. The DOA is acquired easily by recording the entire process of the blue shifting and photobleaching of QDs aggregates. First-order spectrum of each QD in the aggregates can be released from the original overlapped spectral image of the aggregates in sequence under continuous illumination because QDs exhibit the asynchronous spectra blue shifting. Employed 0.3 nM functional QDs in the sensing system, an ultralow detection limit of 4.6 pM was reached by the counting DOA-based sensing strategy. Besides, the sensor also shows high selectivity against other 12 metal ions even at high concentrations. At last, the application of the sensing strategy for river water shows that the real samples can be worked well using this method.
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