Light-Harvesting Fluorescent Spherical Nucleic Acids Self-Assembled from a DNA-Grafted Conjugated Polymer for Amplified Detection of Nucleic Acids

The ultralow concentration of nucleic acids in complex biological samples requires fluorescence probes with high specificity and sensitivity. Herein, a new kind of spherical nucleic acids (SNAs) is developed by using fluorescent pi-conjugated polymers (FCPs) as a light-harvesting antenna to enhance the signal transduction of nucleic acid detection. Specifically, amphiphilic DNA-grafted FCPs are synthesized and self-assemble into FCP-SNA structures. Tuning the hydrophobicity of the graft copolymer can adjust the size and light-harvesting capability of the FCP-SNAs. We observe that more efficient signal amplification occurs in larger FCP-SNAs, as more chromophores are involved, and the energy transfer can go beyond the Forster radius. Accordingly, the optimized FCP-SNA shows an antenna effect of up to 37-fold signal amplification and the limit of detection down to 1.7 pM in microRNA detection. Consequently, the FCP-SNA is applied to amplified in situ nucleic acid detecting and imaging at the single-cell level.

Automated summary

In this study, a new type of spherical nucleic acids (SNAs) was developed by using fluorescent pi-conjugated polymers (FCPs) as light-harvesting antennas to enhance signal transduction in nucleic acid detection. The hydrophobicity of the graft copolymer was adjusted to control the size and light-harvesting capability of the FCP-SNAs. The optimized FCP-SNA showed a 37-fold signal amplification effect and a limit of detection as low as 1.7 pM in microRNA detection. This method was successfully applied for amplified in situ nucleic acid detection and imaging at the single-cell level.