Optical probes operating in the second near-infrared window (NIR-II, 1,000-1,700 nm), where tissues are highly transparent, have expanded the applicability of fluorescence in the biomedical field. NIR-II fluorescence enables deep-tissue imaging with micrometric resolution in animal models, but is limited by the low brightness of NIR-II probes, which prevents imaging at low excitation intensities and fluorophore concentrations. Here, we present a new generation of probes (Ag 2 S superdots) derived from chemically synthesized Ag 2 S dots, on which a protective shell is grown by femtosecond laser irradiation. This shell reduces the structural defects, causing an 80-fold enhancement of the quantum yield. PEGylated Ag 2 S superdots enable deep-tissue in vivo imaging at low excitation intensities (<10 mW cm −2) and doses (<0.5 mg kg −1), emerging as unrivaled contrast agents for NIR-II preclinical bioimaging. These results establish an approach for developing superbright NIR-II contrast agents based on the synergy between chemical synthesis and ultrafast laser processing.

Förster resonant energy transfer (FRET) with upconverting nanoparticles (UC-NPs) as donors and quantum dots (QDs) as acceptors has been regarded as a promising tool for biosensing applications. In this work, we use time-resolved fluorescence spectroscopy to analyze the UCNP-to-QD FRET and we focus on the most relevant parameter of the FRET phenomenon, UCNP-QD distance. This distance is controlled by a nanometric silica shell around the UCNP surface. We theoretically reproduce the experimental results applying FRET theory to the distribution of emitting erbium ions in the UCNP. This simple model allows us to estimate the contribution of every erbium 1 ion to the final FRET response and to explore different strategies to improve FRET efficiency. Abbreviations FRET, QD, UCNP KeywordsFörster resonance energy transfer, upconversion, quantum dot

We developed a sensor for the detection of specific microRNA (miRNA) sequences that was based on graphene quantum dots (GQDs) and ssDNA-UCNP@SiO2. The proposed sensor exploits the interaction between the sp2 carbon atoms of the GQD, mainly π–π stacking, and the DNA nucleobases anchored on the upconversion nanoparticles (UCNPs). This interaction brings the GQD to the surface of the ssDNA-UCNP@SiO2 system, enhancing the upconversion emission. On the other hand, hybridization of the single-stranded DNA (ssDNA) chains anchored on the nanoparticles with their complementary miRNA sequences blocks the capacity of the UCNPs to interact with the GQD through π–π stacking. That gives as result a reduction of the fluorescent enhancement, which is dependent on the concentration of miRNA sequences. This effect was used to create a sensor for miRNA sequences with a detection limit of 10 fM.

We report on the quenching-to-enhancement continuous transition of gold-nanoparticle (AuNP) plasmon assisted upconversion (UC) luminescence with increasing AuNP size, as a guideline for the design of optimal sensors based on UCNPs-AuNPs pairs.

We present a sensor that exploits the phenomenon of upconversion luminescence to detect the presence of specific sequences of small oligonucleotides such as miRNAs among others. The sensor is based on NaYF4:Yb,Er@SiO2 nanoparticles functionalized with ssDNA that contain azide groups on the 3′ ends. In the presence of a target sequence, interstrand ligation is possible via the click-reaction between one azide of the upconversion probe and a DBCO-ssDNA-biotin probe present in the solution. As a result of this specific and selective process, biotin is covalently attached to the surface of the upconversion nanoparticles. The presence of biotin on the surface of the nanoparticles allows their selective capture on a streptavidin-coated support, giving a luminescent signal proportional to the amount of target strands present in the test samples. With the aim of studying the analytical properties of the sensor, total RNA samples were extracted from healthy mosquitoes and were spiked-in with a specific target sequence at different concentrations. The result of these experiments revealed that the sensor was able to detect 10–17 moles per well (100 fM) of the target sequence in mixtures containing 100 ng of total RNA per well. A similar limit of detection was found for spiked human serum samples, demonstrating the suitability of the sensor for detecting specific sequences of small oligonucleotides under real conditions. In contrast, in the presence of noncomplementary sequences or sequences having mismatches, the luminescent signal was negligible or conspicuously reduced.