DNA Encountering Terbium(III): A Smart “Chemical Nose/Tongue” for Large-Scale Time-Gated Luminescent and Lifetime-Based Sensing

Abstract

Recent years have witnessed the rapid development of pattern-based sensors due to their potential to detect and differentiate a wealth of analytes with only few probes. However, no one has found or used the combination of DNA and terbium(III) (Tb) as a pattern recognition system for large-scale mix-and-measure assays. Here we report for the first time that DNA-sensitized Tb (DNA/Tb), as a label-free and versatile "chemical nose/tongue", can be employed for wide-scale time-gated luminescent (TGL) monitoring of metal ions covering nearly the entire periodic table in a cost-effective fashion. A series of guanine/thymine (G/T)-rich DNA ligands was screened to sensitize the luminescence of Tb (referring to the antenna effect) as smart pattern responders to metal ions in solution, and metal ion-DNA interactions can differentially alter the antenna effect of DNA toward Tb as pattern signals. Our results show that as few as 3 DNA/Tb label-free sensors could successfully discriminate 49 analytes, including alkali-metal ions, alkaline-earth-metal ions, transition/post-transition metal ions, and lanthanide ions. A blind test with 49 metals further confirmed the discriminating power of DNA/Tb sensors. Moreover, the lifetime-based pattern recognition application using DNA/Tb sensors was also demonstrated. This DNA/Tb pattern recognition strategy could be extended to construct a series of "chemical noses/tongues" for monitoring various biochemical species by using different responsive DNA ligands, thus promising a versatile and powerful tool for a sensing application and investigation of DNA-involving molecular interactions.

Time-space-resolved origami hierarchical electronics for ultrasensitive detection of physical and chemical stimuli

“…The results prove that the canonical resistance-response patterns from the aforesaid VOCs can, respectively, be easily differentiated using our one-sided OHSA at both temperatures. Since the second principle component (PC2) and the third principle component (PC3) of the 3D PCA plots were <40% 13 (Supplementary Fig. 22a), it was reasonable and acceptable to adopt the first principle component (PC1) to depict the pattern of aforesaid VOC samples under different temperatures (Supplementary Fig.…”

“…For this issue, array-based e-nose/e-tongue sensing approaches, analogous to mammalian sensation 11 , would work through discriminating a distinct pattern of responses generated by stimuli, leading to a fingerprint for their recognition. This approach depends on the interactions between multiple reporter elements and the stimuli of interest 12,13 . Typically, a traditional e-nose/e-tongue sensor array has a planar layout of substrate, in which different sensors made from various materials 14 or chemically modified host material 15 are mainly exposed to stimuli within a planar space at the same time.…”

Single‐Component Chemical Nose with a Hemicyanine Probe for Pattern‐Based Discrimination of Metal Ions†

“…[21][22][23] A chemical nose usually combines sensor arrays with statistical data analysis methods to qualitatively and quantitatively detect multiple analytes. [24][25][26][27][28] Optical probes are widely used to form these sensor arrays and generate information-rich crossresponsive signals. By taking advantages of the well-established statistical methods such as principal component analysis (PCA) and hierarchical clustering analysis (HCA), the optical signals could be converted to more discriminate patterns.…”

Luminescent Hydroxyapatite Doped with Rare Earth Elements for Biomedical Applications

“…Terbium is an essential element of the rare earth family that presents complex optical, magnetic, and electronic properties. It is also an appropriate candidate for applications in the glass industry [48,49], information industry [50], polymers [51,52], bio-chemical sensors [53,54,55], and solar cells [56,57,58]. Terbium is unavoidably present in the environment, organisms, and food chains due to its extensive development and utilization.…”