Exciton Energy Transfer-Based Fluorescent Sensing through Aptamer-Programmed Self-Assembly of Quantum Dots

A novel exciton energy transfer-based ultra-sensitive fluorescent sensing strategy for the detection of biological small molecules and protein has been established through split aptamer-programmed self-assembly of quantum dots (QDs). The signal is produced from exciton energy transfer of the self-assembled QDs. The recognition is accomplished using an aptamer sensor scaffold designed with two split fragment sequences, which specifically bind to the model analytes. The extent of particle assembly, induced by the analyte-triggered self-assembly of QDs, leads to an exciton energy transfer effect between interparticles, giving a readily detectable fluorescent quenching and red shift of the emission peak, which enables us to quantitate the target in dual signal modes. The application of the technique is well demonstrated using two representative split aptamer-based model systems for the detection of adenosine and thrombin. The sensitivity of this exciton energy transfer-based fluorescent sensing is much better than that of plasmonic coupling-based colorimetric methods. Limit of detections (LODs) down to 12 nM and 15 pM can be achieved for adenosine and thrombin, respectively. The sensing strategy is proposed as a general platform for robust and specific aptamer target analysis which could be further developed to monitor a wide range of target analytes. The concept and methodology developed in this work shows a good promise in the study of molecular binding events in the biological and medical applications.